3D‐MOF‐Lattice Inspired Programmable Metamaterials Based on Reconfigurable Polyhedral Origami

Metamaterials have attracted significant attention due to their unconventional mechanical properties. However, a major limitation of conventional metamaterials lies in the fixed and uniform microstructures, limiting their ability to realize diverse functionalities. Inspired by the network chemistry of the 3D architectures of metal–organic frameworks (MOFs) crystal networks, a reconfigurable design strategy based on polyhedral origami patterns is proposed. Leveraging intrinsic bifurcation behavior, a set of modular units with tunable stiffness and adjustable Poisson's ratios is developed. Both experimental and theoretical investigations confirm that these modules exhibit diverse mechanical responses, including quasi‐zero, positive stiffness, bistability, and a continuously tunable Poisson's ratio spanning negative to positive values. By assembling modules in desirable modes, a programmable metamaterial network with customizable mechanical performance is presented. This approach provides a versatile platform for designing multifunctional mechanical metamaterials and offers practical value in applications such as advanced shock‐absorbing systems, enhancing versatility and adaptability.