We developed a chemo-mechatronic system comprising a protein‐based hydrogel bound to a low‐profile laminate that transforms when exposed to different aqueous environments. When modified to include more complex geometries, these controllable shape changes can also be used to selectively trigger multiple folding events, illustrating a new platform for chemically initiated mechatronic devices. This work shows how compositionally discrete components are physically, chemically, and mechanically coupled together to generate a new actuator for biohybrid self‐folding systems.

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