Biodegradable elastomeric networks with exceptional shape memory response under physiological temperature stimuli

• Biocompatible hydrophilic (PEG) and hydrophobic (PDMS) segments were employed. • The polymers were easily processible due to comparatively low T trans (50 °C) of PCL segments. • Tensile characterization exhibited exceptional elasticity (break strain > 2,000 %). • Recoverable shape-memory performance shown for in-vitro application. Stimuli-responsive and resilient shape memory polymers (SMPs) were developed to meet burgeoning demands for biomedical applications requiring biodegradable, shape-memory properties with elasticity. However, few studies have been carried out to engineer tunable mechanical properties into SMPs, which are crucial factors for wide applicability. In this study, a series of polyurethane-based elastomer networks derived cross-linked acrylate-terminated tri-block copolymers (BCPs) with varying internal block segment and block weight fraction with polycaprolactone were synthesized and their chemical, physical, surface, and shape-memory properties were characterized and good mechanical property (break strain > 2000 %), reversible shape-memory properties were observed. The strategy reported herein with tailorable hydrophilicity / hydrophobicity and mechanical property can be leveraged to boost the development of stimuli-responsive polymers and smart materials for future biomedical applications.