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Programmable hydrogels are an emerging class of intelligent materials engineered to respond precisely to specific stimuli, offering tailored functionalities with significant potential for biomedical applications, including drug delivery, tissue engineering, and wound healing. This review comprehensively explores various programmable hydrogels responsive to diverse triggers, including temperature, gene expression, color, shape, and mechanical force. The design and fabrication methods underlying these systems are detailed, highlighting the roles of crosslinkers, adhesion groups, and photosensitive functional groups. Furthermore, the key physical, chemical, and biological properties that govern the performance and functionality of hydrogels are analyzed. The review further examines the mechanisms and recent advancements in self‐executing hydrogels, such as self‐activated, self‐oxygenated, self‐expandable, and self‐powered systems, demonstrating how these innovative designs drive the development of next‐generation programmable hydrogels. The main challenges in hydrogel design, including complexity, reproducibility, and clinical translation, are also addressed. Finally, a perspective on future research directions, highlighting the integration of the latest technologies to realize programmable hydrogels with dynamic closed‐loop responsiveness, bionic synergy, and robust clinical applicability, is offered. This review summarizes the design principles and key features of programmable hydrogels that respond to multiple stimuli. It then delves into the cutting‐edge mechanisms of self‐executing systems, highlighting their role as the cornerstone of next‐generation programmable hydrogels (NGPHs). Finally, by addressing critical challenges in complexity and translation, the review looks to the future of NGPHs, emphasizing their evolution toward dynamic closed‐loop control, biomimetic intelligence, and successful clinical integration.

Adhesives have a long and illustrious history throughout human history. The development of synthetic polymers has highly improved adhesions in terms of their strength and environmental tolerance. As soft robotics, flexible electronics, and intelligent gadgets become more prevalent, adhesives with changeable adhesion capabilities will become more necessary. These adhesives should be programmable and switchable, with the ability to respond to light, electromagnetic fields, thermal, and other stimuli. These requirements necessitate novel concepts in adhesion engineering and material science. Considerable studies have been carried out to develop a wide range of adhesives. This review focuses on stimuli‐responsive material‐based adhesives, outlining current research on switchable and controlled adhesives, including design and manufacturing techniques. Finally, the potential for smart adhesives in applications, and the development of future adhesive forms are critically suggested. In this review, the authors focused on stimuli‐responsive materials‐based adhesives, summarizing the current works of switchable and controllable adhesives, including the design and fabrication strategies. Finally, the challenges and opportunities for smart adhesives in applications and future forms of adhesives are discussed.

Shape‐morphing hydrogels bear promising prospects as soft actuators and for robotics. However, they are mostly restricted to applications in the abiotic domain due to the harsh physicochemical conditions typically necessary to induce shape morphing. Here, multilayer hydrogel actuator systems are developed using biocompatible and photocrosslinkable oxidized, methacrylated alginate and methacrylated gelatin that permit encapsulation and maintenance of living cells within the hydrogel actuators and implement programmed and controlled actuations with multiple shape changes. The hydrogel actuators encapsulating cells enable defined self‐folding and/or user‐regulated, on‐demand‐folding into specific 3D architectures under physiological conditions, with the capability to partially bioemulate complex developmental processes such as branching morphogenesis. The hydrogel actuator systems can be utilized as novel platforms for investigating the effect of programmed multiple‐step and reversible shape morphing on cellular behaviors in 3D extracellular matrix and the role of recapitulating developmental and healing morphogenic processes on promoting new complex tissue formation. Multilayered cell‐laden hydrogel actuators (CHAs) are developed to mimic dynamic tissue morphogenesis. The CHAs, which show multiple deformations programmably and controllably, enable defined self‐folding and/or user‐regulated, on‐demand‐folding into specific 3D architectures under physiological conditions. With these multilayered cytocompatible systems, potential applications in the biomedical field, such as morphodynamic tissue engineering, are demonstrated.

Life‐like materials that can dynamically morph their shape/texture, inspired by living organisms such as cephalopods are sought after for soft robotics and camouflage applications. Achieving such functions demands multimaterials with spatially programmed responses, yet their creation remains challenging. The existing approaches have been limited by the specific in situ polymerization conditions, fluidity of the synthetic components, and the complex, multi‐step processing requirements. Here, we propose a universal strategy that enables programming of material response within pre‐synthesized, ready‐to‐use, clickable microgels with different response behaviors. These microgels can be deposited within desired regions of the material structure via direct ink writing to enable pre‐programmed, localized responses to external stimuli. Spontaneous interparticle stabilization of the deposited microgels via a click reaction (Diels‐Alder bonding) yields shape‐stable, free‐form granular hydrogel multimaterials with reversible, repeatable, and spatially selective responses to stimuli (e.g., pH and temperature). The strategy establishes a 4D‐printing‐compatible, scalable modular platform for facile fabrication of soft materials with programmable shape adaptivity. Clickable microgel inks enable direct ink writing of hydrogel architectures with intrinsic spatioselective and programmable multi‐responsiveness. By combining pH‐responsive and temperature‐responsive microgel building blocks through Diels‐Alder interparticle crosslinking, the assemblies exhibit controllable swelling and shape changes. This modular platform illustrates a versatile strategy to design adaptive materials with tunable responses across multiple stimuli.

Hydrogels capable of stimuli-responsive deformation are widely explored as intelligent actuators for diverse applications. It is still a significant challenge, however, to “program” these hydrogels to undergo highly specific and extensive shape changes with precision, because the mechanical properties and deformation mechanism of the hydrogels are inherently coupled. Herein, two engineering strategies are simultaneously employed to develop thermoresponsive poly(N-isopropyl acrylamide) (PNIPAm)-based hydrogels capable of programmable actuation. First, PNIPAm is copolymerized with poly(ethylene glycol) diacrylate (PEGDA) with varying molecular weights and concentrations. In addition, graphene oxide (GO) or reduced graphene oxide (rGO) is incorporated to generate nanocomposite hydrogels. These strategies combine to allow the refined control of mechanical and diffusional properties of hydrogels over a broad range, which also directly influences variable thermoresponsive actuation. It is expected that this comprehensive design principle can be applied to a wide range of hydrogels for programmable actuation.

Tumor‐associated chronic inflammation severely restricts the efficacy of immunotherapy in cold tumors. Here, a programmable release hydrogel‐based engineering scaffold with multi‐stimulation and reactive oxygen species (ROS)‐response (PHOENIX) is demonstrated to break the chronic inflammatory balance in cold tumors to induce potent immunity. PHOENIX can undergo programmable release of resiquimod and anti‐OX40 under ROS. Resiquimod is first released, leading to antigen‐presenting cell maturation and the transformation of myeloid‐derived suppressor cells and M2 macrophages into an antitumor immune phenotype. Subsequently, anti‐OX40 is transported into the tumor microenvironment, leading to effector T‐cell activation and inhibition of Treg function. PHOENIX consequently breaks the chronic inflammation in the tumor microenvironment and leads to a potent immune response. In mice bearing subcutaneous triple‐negative breast cancer and metastasis models, PHOENIX effectively inhibited 80% and 60% of tumor growth, respectively. Moreover, PHOENIX protected 100% of the mice against TNBC tumor rechallenge by electing a robust long‐term antigen‐specific immune response. An excellent inhibition and prolonged survival in PHOENIX‐treated mice with colorectal cancer and melanoma is also observed. This work presents a potent therapeutic scaffold to improve immunotherapy efficiency, representing a generalizable and facile regimen for cold tumors. The delicate and ever‐changing nature of tumor‐associated chronic inflammation adversely affects anticancer immunity efficiency. Herein, a programmable release hydrogel‐based engineering scaffold with multi‐stimulation and reactive oxygen species (ROS)‐response (PHOENIX) is designed to break the chronic inflammatory balance in cold tumors, resulting in enhanced immunotherapy efficiency and represent a generalizable and facile regimen for cold tumor treatment.

The combination of pharmacologic and endoscopic therapies is the gold standard for treating intestinal failures. The possibility of chemical solubility in water is mandatory for intelligent capsules. Functionalised silk fibroin with peptides and covalently linking different molecular entities to its structure make this protein a platform for preparing gels dissolving in the small and large intestine for drug delivery. In the present study, we linked a peptide containing the cell-adhesive motif Arginine–Glycine–Aspartic acid (RGD) to degummed silk fibres (DSF). Regenerated silk fibroin (RS) films obtained by dissolving functionalised DSF in formic acid were used to prepare composite gelatin. We show that such composite gelatin remains stable and elastic in the simulated gastric fluid (SGF) but can dissolve in the small and large intestines’ neutral-pH simulated intestine fluid (SIF). These findings open up the possibility of designing microfabricated and physically programmable scaffolds that locally promote tissue regeneration, thanks to bio-enabled materials based on functionalised regenerated silk.

Post-surgical complications, particularly hemorrhage and tumor recurrence, remain leading drivers of morbidity, extended hospitalization, and healthcare burden. Hemorrhage poses an immediate, life-threatening risk, while tumor recurrence undermines long-term survival and quality of life. Current hemostatic agents—while effective in providing rapid local clot formation—are constrained by poor tissue adherence, mechanical fragility, and limited durability, often necessitating re-intervention. Similarly, conventional adjuvant strategies (e.g., systemic chemotherapy or radiotherapy) fail to achieve adequate drug concentrations at the surgical bed, exposing patients to systemic toxicity while leaving behind residual disease that seeds recurrence. This dual clinical challenge underscores a critical unmet need for multifunctional, localized, and adaptive post-surgical interventions. Programmable DNA hydrogels have recently emerged as next-generation biomaterials uniquely suited to address this gap. Built from sequence-specific DNA motifs that self-assemble into three-dimensional networks, these hydrogels combine biocompatibility and biodegradability with tunable mechanical strength and stimuli-responsive release. Crucially, they can be engineered to carry pro-coagulant agents for immediate hemostasis while simultaneously delivering chemotherapeutics, immunomodulators, or targeted nanoparticles to suppress residual tumor growth. Beyond drug delivery, hybrid DNA hydrogel systems can integrate biosensing elements and smart, patient-specific responsiveness, enabling precision post-operative care. This review provides a clinician-focused overview of DNA hydrogels in surgical oncology. We emphasize their dual-function potential—rapid hemostasis and recurrence prevention—while outlining mechanistic underpinnings, preclinical evidence, and translational pathways. By bridging bioengineering, biomaterials science, and oncology, we propose DNA hydrogels as a roadmap toward next-generation, adaptive therapeutics that redefine post-surgical management. Graphical Abstract Highlights Dual-function therapeutic potential : DNA hydrogels simultaneously promote rapid post-surgical hemostasis and prevent tumor recurrence. Programmable, stimuli-responsive platform : Sequence-specific DNA motifs allow precise spatial and temporal release of chemotherapeutics, immunomodulators, and pro-coagulant factors. Targeted post-operative intervention : Functionalization with ligands, aptamers, or antibodies ensures selective accumulation at surgical sites and residual tumor niches. Integration of bioengineering and biomaterials : Hybrid DNA-polymer and DNA-nanoparticle systems enhance mechanical robustness, drug loading, and site-specific efficacy. Real-time monitoring and adaptive therapy : Biosensor integration enables dynamic assessment of hemostatic progression and residual tumor activity, facilitating precision post-operative care. Translational relevance : DNA hydrogels provide a next-generation platform for patient-specific, multifunctional post-surgical therapeutics, bridging regenerative medicine and oncology.

In this work, an innovative model is proposed as a design tool to predict both the inner and outer radii in rolled structures based on polydimethylsiloxane bilayers. The model represents an improvement of Timoshenko’s formula taking into account the friction arising from contacts between layers arising from rolling by more than one turn, hence broadening its application field towards materials based on elastomeric bilayers capable of large deformations. The fabricated structures were also provided with surface topographical features that would make them potentially usable in different application scenarios, including cell/tissue engineering ones. The bilayer design parameters were varied, such as the initial strain (from 20 to 60%) and the bilayer thickness (from 373 to 93 µm). The model matched experimental data on the inner and outer radii nicely, especially when a high friction condition was implemented in the model, particularly reducing the error below 2% for the outer diameter while varying the strain. The model outperformed the current literature, where self-penetration is not excluded, and a single value of the radius of spontaneous rolling is used to describe multiple rolls. A complex 3D bioinspired hierarchical elastomeric microstructure made of seven spirals arranged like a hexagon inscribed in a circumference, similar to typical biological architectures (e.g., myofibrils within a sarcolemma), was also developed. In this case also, the model effectively predicted the spirals’ features (error smaller than 18%), opening interesting application scenarios in the modeling and fabrication of bioinspired materials.

Recombinant protein hydrogels have emerged as transformative biomaterials that overcome the bioinertness and unpredictable degradation of traditional synthetic systems by leveraging genetically engineered backbones, such as elastin-like polypeptides, SF, and resilin-like polypeptides, to replicate extracellular matrix (ECM) dynamics and enable programmable functionality. Constructed through a hierarchical crosslinking strategy, these hydrogels integrate reversible physical interactions with covalent crosslinking approaches, collectively endowing the system with mechanical strength, environmental responsiveness, and controlled degradation behavior. Critically, molecular engineering strategies serve as the cornerstone for functional precision: domain-directed self-assembly exploits coiled-coil or β-sheet motifs to orchestrate hierarchical organization, while modular fusion of bioactive motifs through genetic encoding or site-specific conjugation enables dynamic control over cellular interactions and therapeutic release. Such engineered designs underpin advanced applications, including immunomodulatory scaffolds for diabetic wound regeneration, tumor-microenvironment-responsive drug depots, and shear-thinning bioinks for vascularized bioprinting, by synergizing material properties with biological cues. By uniting synthetic biology with materials science, recombinant hydrogels deliver unprecedented flexibility in tuning physical and biological properties. This review synthesizes emerging crosslinking paradigms and molecular strategies, offering a framework for engineering next-generation, adaptive biomaterials poised to address complex challenges in regenerative medicine and beyond.