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Abstract Based on computational modeling, the interaction between catalyst-coated surfaces and flexible micro-to-mesoscale two-dimensional (2D) sheets in solution promotes the self-organization of individual sheets into complex three-dimensional (3D) dynamic forms, including intertwined, self-spinning structures, coupled oscillators and motile, shape-shifting layers. These findings can hasten the development of active, reconfigurable interfaces needed for human–machine interactions. Furthermore, one sheet that autonomously reconfigures into multiple 3D shapes is beneficial for manufacturing, reducing the need to fabricate a new structure for each separate application. More generally, because the flexible 2D sheets display greater degrees of freedom than the previously studied hard zero-dimensional and one-dimensional particles, these elastic layers can reveal new, dynamic behavior in chemically active systems. Graphical abstract