Solid‐Phase Molecular Self‐Assembly Enabled Glue‐Free Antifatigue Laminate Programmable Materials

Abstract Repeated programmability has emerged as a desired property in smart device engineering, but the programmability will fatigue upon repeated applications due to the unmatched mechanical property between the layer materials and the polymeric glue that is required to integrate the two individual oriented layers. It is reported here that glue‐free antifatigue programmable laminate materials can be made with films resulted from solid‐phase molecular self‐assembly (SPMSA). The SPMSA films are created by squeezing the precipitates of oppositely charged polyelectrolytes and DTAB with a noodle machine, where the hydrophobic DTAB molecules self‐assembled into wormlike micelles and oriented along the squeezing direction. The surface molecules in this film are endowed with sufficient mobility in the presence of hydration water, so that two such films are able to be pressed into a laminate material owing to the hydrophobic and electrostatic interactions between the molecules on the two adjacent surfaces. As the water evaporated gradually, the left laminate materials are glue‐free with the same composition. When many of such films are integrated with specific designs, complicated shape programming is able to be achieved, and the programmability is reversible without fatigue. The current strategy is envisioned as a potent intriguing pathway leading to advanced programable materials.