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Brush-like elastomers with crystallizable side chains hold promise for biomedical applications requiring the presence of two distinct mechanical states below and above body temperature: hard and supersoft. The hard semicrystalline state facilitates piercing of the body whereupon the material softens to match the mechanics of surrounding soft tissue. To understand the transition between the two states, the crystallization process was studied with synchrotron X-ray scattering for a series of brush elastomers with poly(ε-caprolactone) side chains bearing from 7 to 13 repeat units. The so-called bottlebrush correlation peak was used to monitor configuration of bottlebrush backbones in the amorphous regions during the crystallization process. In the course of crystallization, the backbones are expelled into the interlamellar amorphous gaps, which is accompanied by their conformational changes and leads to partitioning to unconfined (melt) and confined (semicrystalline) (conformational) states. The crystallization process starts by consumption of the unconfined macromolecules by the growing crystals followed by reconfiguration of macromolecules within the already grown spherulites. 

Polymeric networks are commonly used for various biomedical applications, from reconstructive surgery to wearable electronics. Some materials may be soft, firm, strong, or damping however, implementing all four properties into a single material to replicate the mechanical properties of tissue has been inaccessible. Herein, we present the A- g -B brush-like graft copolymer platform as a framework for fabrication of materials with independently tunable softness and firmness, capable of reaching a strength of ∼10 MPa on par with stress-supporting tissues such as blood vessel, muscle, and skin. These properties are maintained by architectural control, therefore diverse mechanical phenotypes are attainable for a variety of different chemistries. Utilizing this attribute, we demonstrate the capability of the A- g -B platform to enhance specific characteristics such as tackiness, damping, and moldability.