The recent decade has witnessed a growing demand to substitute synthetic materials with naturally-derived platforms for minimizing their undesirable footprints in biomedicine, environment, and ecosystems. Among the natural materials, cellulose, the most abundant biopolymer in the world with key properties, such as biocompatibility, biorenewability, and sustainability has drawn significant attention. The hierarchical structure of cellulose fibers, one of the main constituents of plant cell walls, has been nanoengineered and broken down to nanoscale building blocks, providing an infrastructure for nanomedicine. Microorganisms, such as certain types of bacteria, are another source of nanocelluloses known as bacterial nanocellulose (BNC), which benefit from high purity and crystallinity. Chemical and mechanical treatments of cellulose fibrils made up of alternating crystalline and amorphous regions have yielded cellulose nanocrystals (CNC), hairy CNC (HCNC), and cellulose nanofibrils (CNF) with dimensions spanning from a few nanometers up to several microns. Cellulose nanocrystals and nanofibrils may readily bind drugs, proteins, and nanoparticles through physical interactions or be chemically modified to covalently accommodate cargos. Engineering surface properties, such as chemical functionality, charge, area, crystallinity, and hydrophilicity, plays a pivotal role in controlling the cargo loading/releasing capacity and rate, stability, toxicity, immunogenicity, and biodegradation of nanocellulose-based delivery platforms. This review provides insights into the recent advances in nanoengineering cellulose crystals and fibrils to develop vehicles, encompassing colloidal *

conditions to maintain the scale of medical device manufacturing; and 4) the treatment must not incorporate antibiotics to maintain global antimicrobial stewardship efforts. The zwitterionic polymer polysulfobetaine (PSB) was selected as the antifouling component of the surface modification to benefit from its biocompatibility, ultralow-fouling properties, and oxidative stability. By adsorbing water electrostatically, PSB coatings form a thin hydration barrier that prevents organic materials from adhering to surfaces. [22] Commonly used approaches to attach PSB coatings to surfaces, such as radical-initiated graft polymerizations of PSB-methacrylate necessitate the use of oxygen-free conditions, [23] preconditioning steps, [24] or long reaction times [25] that do not meet scalability requirements. To circumvent the use of air-free graft polymerizations, we employ perfluorophenylazide (PFPA) chemistry as a molecular anchor to link the PSB coatings onto the surfaces of polymeric materials under ambient conditions. When triggered with UV-light, PFPA moieties generate a highly reactive nitrene that forms covalent bonds with materials containing amines, CC double bonds, and CH bonds. [26,27] With this method, PSB is rapidly coated onto a broad range of substrates using UV light under ambient conditions with no preconditioning steps. Thus, many different medical devices may be quickly and conveniently treated on the manufacturing level.We first demonstrate the effect of the treatment on polydimethylsiloxane (PDMS) as an exemplary, extremely difficultto-modify model for a common elastomer used in implantable medical devices. [28] Commonly known as silicone, PDMS is widely used for its biocompatibility, good chemical stability, ease of fabrication using injection molding or extrusion, and low cost. [29][30][31] Many implantable device makers have moved away from classical medical elastomers and plastics such as latex and polyvinyl chloride due to allergens [32] or plasticizers [33] in these materials that leach out and often lead to irritation or complications. PDMS-based devices do not require plasticizers and have been shown to lead to fewer complications than latex and polyurethane-based devices. [34] Despite its ideal properties, the nonpolar nature of PDMS facilitates the adhesion of organic materials. Bacteria, platelets, proteins, and other biomolecules bind strongly to the hydrophobic surfaces of PDMS elastomers, leading to the colonization and proliferation of biofilms. [22] When common hydrophilic surface treatments are performed on PDMS, such as plasma oxidation, [35] UV-ozone, [36] or corona discharge, [37] the effects are short-term due to rapid hydrophobic recovery. The highly mobile chains of PDMS (glass transition temperature ≈ −120 °C) can reorient themselves to "hide" the surface modified elastomers, when exposed to air, within hours. [38] Other methods seeking long-lasting hydrophilic PDMS surfaces typically require preconditioning steps with silane [39][40][41] chemistry or radical polymerization. [...

Harmful microbes can grow freely on implanted medical devices such as catheters (as shown on the right). In article number 2200254, Amir Sheikhi, Richard B. Kaner, and coworkers, report a new method to apply a robust surface coating containing zwitterions, which creates a water layer that prevents biofilm formation (as shown on the left). This can improve the safety of the medical devices and reduce patient complications. Image credit: Amir Sheikhi/Penn State.