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Surface functionalization of an implantable device with bioactive molecules can overcome adverse biological responses by promoting specific local tissue integration. Bioactive peptides have advantages over larger protein molecules due to their robustness and sterilizability. Their relatively small size presents opportunities to control the peptide orientation on approach to a surface to achieve favourable presentation of bioactive motifs. Here we demonstrate control of the orientation of surface-bound peptides by tuning electric fields at the surface during immobilization. Guided by computational simulations, a peptide with a linear conformation in solution is designed. Electric fields are used to control the peptide approach towards a radical-functionalized surface. Spontaneous, irreversible immobilization is achieved when the peptide makes contact with the surface. Our findings show that control of both peptide orientation and surface concentration is achieved simply by varying the solution pH or by applying an electric field as delivered by a small battery. Implanted materials can be rejected by the body, and coating the surfaces with peptides is seen as an option to overcome this problem. Here, the authors investigated how pH and electric fields can be used to prepare defined peptide coatings.

AlCrFeCoNiCu 0.5 thin films were fabricated by cathodic arc deposition under different substrate biases. Detailed characterization of the chemistry and structure of the film, from the substrate interface to the film surface, was achieved by combining high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, and atomic force microscopy. Computer simulations using the transport of ions in matter model were applied to understand the ion surface interactions that revealed the key mechanism of the film growth. The final compositions of the films are significantly different from that of the target used. A trend of elemental segregation, which was more pronounced with higher ion kinetic energy, was observed. The XPS results reveal the formation of Al 2 O 3 and Cr 2 O 3 on the thin film surface. The grain size is shown to increase with the increasing of the ion kinetic energy. The growth of equiaxed grains contributed to the formation of a flat surface with a relatively low surface roughness as shown by atomic force microscopy.

Adverse body reactions to blood-contacting medical devices endanger patient safety and impair device functionality, with events invariably linked to nonspecific protein adsorption due to suboptimal material biocompatibility. To improve the safety and durability of such devices, herein we propose a strategy for introducing stable zwitterionic grafts onto polymeric surfaces via plasma functionalization. The resulting zwitterion-grafted substrates exhibit long-lasting superhydrophilicity, enabling antifouling and anti-thrombogenic properties. We demonstrate the successful modification of the surface elemental composition, morphology, and hydrophilicity, while retaining the underlying mechanical properties of the polymeric substrate. Furthermore, we optimise the fabrication process to ensure long-lasting modifications at least three months after fabrication. This strategy decreases fibrinogen adsorption by approximately 9-fold, and thrombosis by almost 75% when applied to a commercial polyurethane. Moreover, this process is universally applicable to a wide range of polymeric materials, even those with stable chemistry such as polytetrafluoroethylene.Poor material biocompatibility of implanted medical devices endangers patient safety and impairs device functionality. Here, durable zwitterion grafts attached onto polymeric surfaces via plasma functionalization lead to superhydrophilic materials for safer and more durable devices.

Dental implants are the primary solution for tooth replacement, providing both aesthetic and functional restoration. Their long-term success depends not only on osseointegration but also on robust peri-implant soft tissue integration (PSTI), particularly in the transmucosal region, where a stable epithelial seal is critical to preventing microbial infiltration and peri-implant inflammation. While surface topography modifications such as roughness, morphology, and porosity influence gingival cell behavior, passive surface modifications alone are often insufficient to promote rapid PSTI. This raises a fundamental question in dental implant design: How can implant surfaces be bioengineered to actively promote PSTI rather than passively relying on cellular responses? This review examines how biofunctionalization has emerged as a transformative strategy in implant surface engineering and critically analyses the latest biofunctionalization strategies for dental implants, with a particular focus on the underlying mechanisms that regulate biomolecule-implant interactions. It evaluates biomolecule incorporation via physical and covalent attachment, highlighting their distinct advantages in stability, efficiency, and scalability. We discuss approaches for functionalizing dental implant surfaces with bioactive molecules, such as proteins and peptides, and cells to replicate natural biological interactions, regulate immune responses, and enhance antimicrobial defense mechanisms. By addressing how bioengineered surfaces can be designed to actively engage with biological systems, this review provides a framework for developing next-generation implant technologies that achieve more effective and predictable PSTI, with strong potential for clinical translation. [Display omitted] •A critical and mechanistically focused review of biomolecule-functionalized dental implants, with specific emphasis on strategies to enhance soft tissue integration and epithelial sealing.•Systematically evaluates both physical and covalent biomolecule immobilization techniques, comparing their stability, scalability, and biological effectiveness for clinical translation.•Bridges biomaterials science and biology by dissecting the molecular mechanisms by which immobilized biomolecules modulate cell adhesion, immune responses, and inflammation resolution at the implant–tissue interface.•Identifies current limitations and overlooked challenges in long-term coating performance, biomolecule stability, and reproducibility of functionalization techniques under physiological conditions.•Outlines a roadmap for the development of next-generation bioactive dental implants with enhanced soft tissue integration, highlighting opportunities for multi-agent loading, stimuli-responsive surfaces, and scalable plasma-enabled fabrication strategies.

Covalent biofunctionalization of implant surfaces using anti microbial agents is a promising approach to reducing bone infection and implant failure. Radical‐rich, ion‐assisted plasma polymerized (IPP) coatings enable surface covalent biofunctionalization in a simple manner; but until now, they are limited to only 2D surfaces. Here a new technology is demonstrated to create homogenous IPP coatings on 3D materials using a rotating, conductive cage that is negatively biased while immersed in RF plasma. Evidence is provided that under controlled energetic ion bombardment, this technology enables the formation of highly robust and homogenous radical‐rich coatings on 3D objects for subsequent covalent attachment of antimicrobial agents. To functionally apply this technology, the broad‐spectrum antimicrobial CSA‐90 is attached to the surfaces, where it retained potent antibacterial activity against Staphylococcus aureus. CSA‐90 covalent functionalization of stainless‐steel pins used in a murine model of orthopedic infection revealed the highly promising potential of this coating system to reduce S. aureus infection‐related bone loss. This study takes the previous research on plasma‐based covalent functionalization of 2D surfaces a step further, with important implications for ushering in a new dimension in the biofunctionalization of 3D structures for applications in bone implants and beyond. A plasma‐based technology to create anti‐infection bone implants is introduced. It enables the creation of robust coatings rich in radicals, facilitating strong attachment of antimicrobial agents through covalent bonding. The solvent‐free biofunctionalization, tailored for 3D materials, streamlines functional biomaterial fabrication. It holds promise for efficient development of antibacterial and tissue‐integrating implants.

Plasma polymerization enables rapid, solvent‐free synthesis of polymeric nanoparticles (PPNs) bearing long‐lived reactive radicals, which create a highly functionalized interface enabling single‐step covalent attachment of diverse molecules. A major barrier to translation, however, is the limited understanding of how storage conditions affect physicochemical stability and functionality. Here, it is demonstrated that PPNs retain exceptional physicochemical stability while retaining their functionality as nanocarrier when stored under optimized conditions. Dry‐phase storage at ambient temperature maintained a stable hydrodynamic size (207 ± 3.1 nm) and preserved 62.0 ± 2.0% of the initial radical concentration over 12 weeks, with no measurable changes in elemental composition or chemical bonding, confirmed by dynamic light scattering (DLS), electron paramagnetic resonance (EPR) spectroscopy, and X‐ray photoelectron spectroscopy (XPS). Even after one year of storage, aged PPNs exhibited equivalent interfacial reactivity to freshly prepared particles, evidenced by efficient covalent conjugation with Nile Blue, highlighted through fluorescence spectroscopy, attenuated total reflectance – Fourier transform infrared spectroscopy (ATR‐FTIR), and XPS. Intracellular uptake studies revealed that functionalized PPNs with aged cores retained bioactivity, exhibiting internalization in A549 lung cancer cells comparable to freshly synthesized counterparts. These findings establish key parameters for preserving PPN surface reactivity and biofunctionality, offering important design guidelines for long‐term storage. Plasma polymerized nanoparticles (PPNs) offer a solvent‐free route to functional nanocarriers with long‐lived radicals. This study establishes design principles for long‐term storage of PPNs, demonstrating that dry‐phase storage retains radical content, covalent reactivity, and bioactivity over extended periods. These findings advance the translational potential of plasma‐engineered nanomaterials.

Bone is a structurally complex and dynamic tissue that plays a crucial role in mobility and skeletal stability. However, conditions such as osteoporosis, osteoarthritis, trauma-induced fractures, infections, and malignancies often necessitate the use of orthopedic and dental implants. Despite significant progress in implant biomaterials, challenges such as bacterial infection, inflammation, and loosening continue to compromise implant longevity, frequently leading to revision surgeries and extended recovery times. Smart coatings have emerged as a next-generation solution to these problems by providing on-demand, localized therapeutic responses to microenvironmental changes around implants and promoting bone regeneration. Such coatings can minimize antibiotic resistance by enabling controlled, stimulus-triggered drug release. Although the idea of using pH-sensitivity as a tool to make smart coatings is not a new thought, there are no options currently good enough to enter clinical studies. This review provides a comprehensive overview of recent advances in pH-sensitive polymers, hybrid composites, porous architectures, and bioactive linkers designed to dynamically respond to pathological pH variations at implant sites. By investigating the mechanisms of action, antibacterial and anti-inflammatory effects, and roles in bone regeneration, it is shown that the ability to provide time-dependent drug release for both short-term and long-term infections, as well as keeping the environment welcoming to the bone cell growth and replacement, is not an easy goal to reach, even with a fully biocompatable, non-toxic, and semi-biodegradable (one that releases the drug, but does not fade away) coating material compound. Reviewing all available options, including their functions and failures, finally, emerging trends, translational barriers, and future opportunities for clinical implementation are highlighted, underscoring the transformative potential of bioresponsive coatings in orthopedic and dental implant technologies.

Osteosarcoma (OS) is a primary malignant bone tumor often treated by surgical resection and systemic chemotherapy, which can cause severe side effects and nonspecific drug distribution. Localized drug delivery via bone scaffolds offers a promising alternative but faces limitations such as poor drug retention, instability of therapeutics, and insufficient mechanical strength for bone repair. This study presents a multifunctional implant integrating doxorubicin (DOX)‐loaded liposomes into Baghdadite (Ca 3 ZrSi 2 O 9 , BAG) ceramics. Ion‐assisted plasma polymer (IPP) coating was employed to enhance liposome immobilization and control DOX release. BAG functionalized with DOX‐loaded liposomes (BAG/DOXlipo) significantly reduced OS cell viability, with enhanced efficacy observed in IPP‐coated samples. Notably, BAG/DOXlipo (with or without IPP) showed no cytotoxicity to human osteoblasts, supported sustained ion release, and promoted alkaline phosphatase activity and bone mineralization. Additionally, the BAG/DOXlipo system demonstrated antibacterial activity against common implant‐related pathogens. This platform uniquely combines mechanical robustness, osteoconductivity, and covalently bound liposomal chemotherapeutics to achieve localized tumor inhibition, bone regeneration, and infection control. It offers a promising strategy for OS treatment while minimizing systemic toxicity.

Achieving robust, cytocompatible bonding of hydrogels to solid substrates remains a long‐lasting challenge in the development of hybrid solid–hydrogel (HSH) systems for biomedical applications. Current strategies for hydrogel–solid bonding suffer from the complexity of processes, toxicity from residual crosslinkers, and substrate dependency; issues that hinder clinical adoption of HSH structures (HSHs). Overcoming these impediments, a dry, reagent‐free strategy is presented to create radical‐rich interlayers that enable initiator‐ and crosslinker‐free covalent attachment of hydrogels for the fabrication of robust HSHs. Evidence is provided in which long‐lived radicals embedded in ion‐assisted plasma polymerized coatings simultaneously drive hydrogel anchoring and in situ crosslinking on diverse non‐polymeric substrates, including titanium, stainless steel, and glass. GelMA, chitosan, and PVA‐Tyr hydrogels are immobilized with high stability, with coatings remaining intact after two months in aqueous media. Tuning the substrate bias voltage modulates radical concentration, enabling precise control over hydrogel thickness and crosslinking density with no need for extra reagents and/or crosslinkers. Cytocompatibility is confirmed with human mesenchymal stem cells and macrophages, with negligible inflammatory activation detected under the tested conditions. To showcase one application among many, fibroblasts on GelMA‐based HSHs exhibited enhanced early attachment, spreading, and proliferation, supporting their application in promoting soft tissue integration. This substrate‐independent, additive‐ and initiator‐free strategy embodies high‐quality‐by‐design principles, enabling a universal and scalable platform for the fabrication of HSH systems, particularly suited for applications requiring seamless integration between soft and hard materials, such as biomedical coatings, tissue‐interfacing constructs, and next‐generation soft robotics.