Programmable Shape Recovery Onset Temperatures via Phase‐Separated Dual‐Network Polymers

ABSTRACT Shape memory polymers (SMPs) are promising for soft robotics and artificial muscles, yet their applicability is largely limited by their recovery onset temperature ( T on ). However, conventional T on regulation relies on compositional changes or complex post‐treatments, hindering the integration of multiple, precisely defined T on within one system. Here, we present a simple strategy to continuously tune T on (28°C–85°C) by controlling phase structures in chemical fixed dual‐network polymers via polymerization‐induced phase separation (PIPS). Furthermore, digital light processing (DLP) enables spatial programming of T on within a single material, allowing the fabrication of fiber actuators with programmable energy release, exhibiting a fourfold difference in release rate and stable performance over 120 cycles. This work provides a new route for designing SMP‐based intelligent actuators, soft robotics, and adaptive systems.