Development of Healable, Recyclable, and Reprocessable Two‐Way Responsive Shape Memory Epoxy Resin Composite Materials

ABSTRACT This work aims to develop a low‐cost, two‐way shape memory composite material with a low‐temperature response, utilizing a polyethylene glycol‐modified thermoplastic epoxy resin/zinc oxide film (EPP‐Z) as the active response layer and a thermosetting epoxy resin/zinc oxide film (EP‐Z) as the passive response layer. The shape memory EPP‐Z/EP‐Z bilayer composite film (PZ/Z) was fabricated through a straightforward lamination technique. Leveraging the response discrepancy between the active and passive layers during heating, the developed PZ/Z exhibits superior two‐way shape memory capability, achieving a maximum two‐way recovery angle of 15°. Notably, PZ/Z operates at a relatively low response temperature, enabling thermal bending at around 40°C and cold recovery at approximately 25°C. Furthermore, the active response layer of PZ/Z was healable, recyclable, and reprocessable. This work provides an innovative process reference for the cost‐effective development of low‐temperature responsive, two‐way shape memory composite materials.