Article states that thiol-ene/acrylate shape memory polymers (SMPs) have sufficient stiffness for facile insertion and precision placement and soften after exposure to physiological conditions to reduce the mechanical mismatch with body tissue; as a result, they have demonstrated excellent potential as substrates for various flexible bioelectronic devices, such as cochlear implants, nerve cuffs, cortical probes, plexus blankets, and spinal cord stimulators. Here, the authors report a new strategy for designing SMPs with enhanced shape recovery properties and lower moduli than previously reported SMPs under physiological conditions without sacrificing stiffness at room temperature by introducing a hydrophilic monomer.