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Hydrogels with tailor‐made swelling‐shrinkable properties have aroused considerable interest in numerous biomedical domains. For example, as swelling is a key issue for blood and wound extrudates absorption, the transference of nutrients and metabolites, as well as drug diffusion and release, hydrogels with high swelling capacity have been widely applicated in full‐thickness skin wound healing and tissue regeneration, and drug delivery. Nevertheless, in the fields of tissue adhesives and internal soft‐tissue wound healing, and bioelectronics, non‐swelling hydrogels play very important functions owing to their stable macroscopic dimension and physical performance in physiological environment. Moreover, the negative swelling behavior (i.e., shrinkage) of hydrogels can be exploited to drive noninvasive wound closure, and achieve resolution enhancement of hydrogel scaffolds. In addition, it can help push out the entrapped drugs, thus promote drug release. However, there still has not been a general review of the constructions and biomedical applications of hydrogels from the viewpoint of swelling‐shrinkable properties. Therefore, this review summarizes the tactics employed so far in tailoring the swelling‐shrinkable properties of hydrogels and their biomedical applications. And a relatively comprehensive understanding of the current progress and future challenge of the hydrogels with different swelling‐shrinkable features is provided for potential clinical translations.

Rapid advances in wearable electronics and mechno‐sensational human–machine interfaces impose great challenges in developing flexible and deformable tactile sensors with high efficiency, ultra‐sensitivity, environment‐tolerance, and self‐sustainability. Herein, a tactile hydrogel sensor (THS) based on micro‐pyramid‐patterned double‐network (DN) ionic organohydrogels to detect subtle pressure changes by measuring the variations of triboelectric output signal without an external power supply is reported. By the first time of pyramidal‐patterned hydrogel fabrication method and laminated polydimethylsiloxane (PDMS) encapsulation process, the self‐powered THS shows the advantages of remarkable flexibility, good transparency (≈85%), and excellent sensing performance, including extraordinary sensitivity (45.97 mV Pa−1), fast response (≈20 ms), very low limit of detection (50 Pa) as well as good stability (36 000 cycles). Moreover, with the LiBr immersion treatment method, the THS possesses excellent long‐term hyper anti‐freezing and anti‐dehydrating properties, broad environmental tolerance (−20 to 60 °C), and instantaneous peak power density of 20 µW cm−2, providing reliable contact outputs with different materials and detecting very slight human motions. By integrating the signal acquisition/process circuit, the THS with excellent self‐power sensing ability is utilized as a switching button to control electric appliances and robotic hands by simulating human finger gestures, offering its great potentials for wearable and multi‐functional electronic applications. Triboelectric hydrogel tactile sensor is constructed based on micro‐pyramid‐patterned DN ionic organohydrogels with two working principles. This self‐powered tactile sensor with wide environmental tolerance and excellent sensing performance is obtained with a subtle immersion treatment and a micro‐pyramid‐patterned method. Combining with a signal acquisition/process circuit, wearable electronics and human–machine interface applications are demonstrated.

Since the last few decades, the development of smart hydrogels, which can respond to stimuli and adapt their responses based on external cues from their environments, has become a thriving research frontier in the biomedical engineering field. Nowadays, drug delivery systems have received great attention and smart hydrogels can be potentially used in these systems due to their high stability, physicochemical properties, and biocompatibility. Smart hydrogels can change their hydrophilicity, swelling ability, physical properties, and molecules permeability, influenced by external stimuli such as pH, temperature, electrical and magnetic fields, light, and the biomolecules’ concentration, thus resulting in the controlled release of the loaded drugs. Herein, this review encompasses the latest investigations in the field of stimuli-responsive drug-loaded hydrogels and our contribution to this matter.

[This corrects the article DOI: 10.1371/journal.pone.0155625.].

The design of new hemostatic materials to mitigate uncontrolled bleeding in emergencies is challenging. Chitosan-based hemostatic hydrogels have frequently been used for hemostasis due to their unique biocompatibility, tunable mechanical properties, injectability, and ease of handling. Moreover, chitosan (CS) absorbs red blood cells and activates platelets to promote hemostasis. Benefiting from these desired properties, the hemostatic application of CS hydrogels is attracting ever-increasing research attention. This paper reviews the recent research progress of CS-based hemostatic hydrogels and their advantageous characteristics compared to traditional hemostatic materials. The effects of the hemostatic mechanism, effects of deacetylation degree, relative molecular mass, and chemical modification on the hemostatic performance of CS hydrogels are summarized. Meanwhile, some typical applications of CS hydrogels are introduced to provide references for the preparation of efficient hemostatic hydrogels. Finally, the future perspectives of CS-based hemostatic hydrogels are presented.

Fast advances in polymer science have provided new hydrogels for applications in drug delivery. Among modern drug formulations, polymeric type stimuli-responsive hydrogels (SRHs), also called smart hydrogels, deserve special attention as they revealed to be a promising tool useful for a variety of pharmaceutical and biomedical applications. In fact, the basic feature of these systems is the ability to change their mechanical properties, swelling ability, hydrophilicity, or bioactive molecules permeability, which are influenced by various stimuli, particularly enzymes. Indeed, among a great number of SHRs, enzyme-responsive hydrogels (ERHs) gain much interest as they possess several potential biomedical applications (e.g., in controlled release, drug delivery, etc.). Such a new type of SHRs directly respond to many different enzymes even under mild conditions. Therefore, they show either reversible or irreversible enzyme-induced changes both in chemical and physical properties. This article reviews the state-of-the art in ERHs designed for controlled drug delivery systems (DDSs). Principal enzymes used for biomedical hydrogel preparation were presented and different ERHs were further characterized focusing mainly on glucose oxidase-, β-galactosidase- and metalloproteinases-based catalyzed reactions. Additionally, strategies employed to produce ERHs were described. The current state of knowledge and the discussion were made on successful applications and prospects for further development of effective methods used to obtain ERH as DDSs.

Gelatin methacryloyl (GelMA) is a versatile material for a wide range of bioapplications. There is an intense interest in developing effective chemical strategies to prepare GelMA with a high degree of batch-to-batch consistency and controllability in terms of methacryloyl functionalization and physiochemical properties. Herein, we systematically investigated the batch-to-batch reproducibility and controllability of producing GelMA (target highly and lowly substituted versions) via a one-pot strategy. To assess the GelMA product, several parameters were evaluated, including the degree of methacryloylation, secondary structure, and enzymatic degradation, along with the mechanical properties and cell viability of GelMA hydrogels. The results showed that two types of target GelMA with five batches exhibited a high degree of controllability and reproducibility in compositional, structural, and functional properties owing to the highly controllable one-pot strategy.

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.

Hydrogels are hydrophilic polymer materials that can swell but are insoluble in water. Hydrogels can be synthesized with synthetic or natural polymers, but natural polymers are preferred because they are similar to natural tissues, which can absorb a high water content, are biocompatible, and are biodegradable. The three-dimensional structure of the hydrogel affects its water insolubility and ability to maintain its shape. Cellulose hydrogels are preferred over other polymers because they are highly biocompatible, easily accessible, and affordable. Carboxymethyl cellulose sodium (CMCNa) is an example of a water-soluble cellulose derivative that can be synthesized using natural materials. A crosslinking agent is used to strengthen the properties of the hydrogel. Chemical crosslinking agent is used more often than physical crosslinking agent. In this review, article, different types of crosslinking agents are discussed based on synthetic and natural crosslinking agents. Hydrogels that utilize synthetic crosslinking agent have advantages, such as adjustable mechanical properties and easy control of the chemical composition. However, hydrogels that use natural crosslinking agent have better biocompatibility and less latent toxic effect.