Thermoset polymers cross-linked by dynamic covalent bonds are recyclable and reconfigurable based on solid-state plasticity, resulting in less waste and environmental pollution. However, most thermoset polymers previously reported show thermal-responsive solid-state plasticity, depending much on external conditions and not allowing for local shape modulation. Herein, the isocyanate modified carbon nanotubes (CNTs-NCO) are introduced into the polythiourethane (PCTU) network with multiple dynamic covalent bonds by in situ polymerization to prepare the composite with thermal/light dual-responsive solid-state plasticity, reconfigurability, and recyclability. The introduction of CNTs-NCO simultaneously strengthens and toughens the PCTU composite. Moreover, based on the photothermal properties and light-responsive solid-state plasticity, the PCTU/CNTs composite or bilayer sample can achieve complex permanent shape by locally precise shape regulation without affecting other parts. This work provides a simple and reliable method for preparing high-performance polymer composite with light-responsive solid-state plasticity, which may be applied in the fields of sensing and flexible electronics.