Protein‐Polymer Dynamic Hydrogels Utilizing Native Ligand Binding for Injectable Therapeutic Delivery and 3D Printing

Dynamic hydrogels comprising networks formed from reversible interactions have shown utility in minimally invasive delivery of encapsulated therapeutics, as well as in extrusion-based 3D printing of tissue-mimetic structures. Here, we report dynamic nanocolloidal hydrogels formed from the co-assembly of spheroidal hyperbranched poly(glycerol) (HPG) and soluble albumin nanoparticles (SANs). Functionalization of the HPG with palmitate (a natural ligand of serum albumin) appears to enable self-association of the HPG, as well as its interaction with SANs, to form dynamic networks. The properties of these networks can be tuned by modifying the size of the SAN in addition to other formulation parameters. To highlight the utility of these dynamic hydrogels, we demonstrate (i) in vitro and in vivo release of a model protein therapeutic from these injectable materials, (ii) preliminarily evaluate biocompatibility of these materials in a murine model, and (iii) demonstrate extrusion-based 3D printing using these materials.