A Facile and General Approach to Recoverable High‐Strain Multishape Shape Memory Polymers

Fabricating a single polymer network with no need to design complex structures to achieve an ideal combination of tunable high‐strain multiple‐shape memory effects and highly recoverable shape memory property is a great challenge for the real applications of advanced shape memory devices. Here, a facile and general approach to recoverable high‐strain multishape shape memory polymers is presented via a random copolymerization of acrylate monomers and a chain‐extended multiblock copolymer crosslinker. As‐prepared shape memory networks show a large width at the half‐peak height of the glass transition, far wider than current classical multishape shape memory polymers. A combination of tunable high‐strain multishape memory effect and as high as 1000% recoverable strain in a single chemical‐crosslinking network can be obtained. To the best of our knowledge, this is the first thermosetting material with a combination of highly recoverable strain and tunable high‐strain multiple‐shape memory effects.