Nanomaterials as Building Blocks in Functional Biomaterials Design

Engineering responsive biomaterials from reversible interactions enables the design of injectable drug delivery platforms and materials for 3D bioprinting. Among the emerging motifs to assemble these materials, polymer–nanoparticle interactions have been introduced as a useful strategy to assemble polymer–nanoparticle materials. In this approach, engineered nanoparticles are used as constituent building blocks in the material design, allowing for a broad range of functionality in biomaterials design. In this presentation, we will describe our efforts in the design of polymer–nanoparticle hydrogels as bioinks for 3D printing. We designed a universal carrier ink composed of PEGylated polymer nanoparticles, cellulose derivatives, and a range of secondary polymers. The rheology enables extrusion-based printing, and the inclusion of secondary polymers provides a strategy for stabilization of the printed constructs. This strategy has been applied in the design of printed constructs for tissue engineering and multimodal drug delivery. In addition, we have advanced this platform by including a supramolecular binding motif based on polypseudorotoxane formation of alpha-cyclodextrin (aCD) on the surface of the PEGylated nanoparticles. This approach enabled tunable mechanical properties as well as modular design of polymer–nanoparticle hydrogels via exchange of the nanoparticles and polymers. Supramolecular reinforcement of polymer–nanoparticles further expanded the scope of applications, including the design of injectable materials for sustained biomolecule release.