Autonomous Folding of Soft Matter From Living Polymers.
Origami provides a versatile framework for shape-morphing, yet existing systems are limited to transitions between an initial state and a predetermined folding outcome, offering little tunability after fabrication. Here we introduce a dynamic "living" polymer that continuously remodels its main-chain network through a growth process, enabling post-fabrication control over size, mechanical properties, and geometry. Incorporated as active crease layers, these polymers drive autonomous folding when supplied with "nutrient solutions" containing monomers, crosslinkers and catalysts. The associated dihedral angles are determined by growth kinetics and crease composition. Iterative regrowth reprograms folding pathways and increases mechanical stiffness up to 50 times. We demonstrate rigid (Miura) and non-rigid patterns (square-twist) that can be repeatedly reconfigured. Through this work, we establish a foundation for adaptive structures with unlimited re-programmability, opening avenues for applications in biomedical wearable devices and multifunctional deployable systems.