Engineering adaptive self-healing biomaterials from jammed microfluidic elastomeric particles

Biomaterials designed for implantation must accommodate the dynamic mechanical and structural environment of the human body. Yet, current strategies for creating materials capable of adapting their shape post-implantation remain limited. In this work, we introduced a remoldable, biodegradable, and biocompatible granular scaffold composed of monodisperse poly(octamethylene maleate (anhydride) citrate) (POMaC) particles. Monodisperse POMaC droplets with controlled diameters were generated using a droplet microfluidic platform, then subsequently jammed and UV-crosslinked to form interconnected, porous, and self-healing elastomeric scaffolds. The scaffold chemical composition and crosslinking parameters directly influenced mechanical properties, stability, and permeability, enabling tunability across a range of tissue engineering applications. The granular scaffold exhibited autonomous self-healing, enhanced molecular diffusivity, and robust cell infiltration, while remaining moldable into prescribed geometries under both in vitro and in vivo conditions. Notably, following implantation, the granular scaffolds could be remolded in vivo 24 h post-implantation, allowing adaptation to a desired geometry while preserving structural integrity, promoting the recruitment of pro-reparative macrophages, and facilitating vascular ingrowth. Collectively, this work established a versatile strategy for designing adaptive implantable biomaterials capable of responding to the body's dynamic environment, with broad potential applications in regenerative medicine and tissue engineering.