Although the potential of layered metal/organic hybrid material has long been recognized, manufacturing analogous materials in large-scale remains extremely difficult owing to the lack of a suitable fabrication process. Here, a top–down approach that combines accumulative roll
bonding technique with selective etching and vacuum impregnation process was first developed to fabricate bulk layered Ta/polymer hybrid material with controlled layer thickness (h) of 100 μm ≥ h ≥ 1 μm. This approach can be generalized to fabricate other layered
metal/polymer hybrid material with a large number of material combinations and a wide range of layer dimensions. This kind of material, which is comprised of hard and soft phases arranged in complex hierarchical architectures, has potential for application as lightweight and energy absorption
structural materials.