Engineering Covalent Organic Frameworks with Polyethylene Glycol as Self‐Sustained Humidity‐Responsive Actuators

Abstract Regarding the global energy crisis, it is of profound significance to develop spontaneous power generators that harvest natural energy. Fabricating humidity‐responsive actuators that can conduct such energy transduction is of paramount importance. Herein, we incorporate covalent organic frameworks with flexible polyethylene glycol to fabricate rigid‐flexible coupled membrane actuators. This strategy significantly improves the mechanical properties and humidity‐responsive performance of the actuators, meanwhile, the existence of ordered structures enables us to unveil the actuation mechanism. These high‐performance actuators can achieve various actuation applications and exhibit interesting self‐oscillation behavior above a water surface. Finally, after being coupled with a piezoelectric film, the bilayer device can spontaneously output electricity over 2 days. This work paves a new avenue to fabricate rigid‐flexible coupled actuators for self‐sustained energy transduction.