▎ 摘　　要

Three-dimensional (3D) architectures of graphene are of great interest for applications in flexible electronics, supercapacitors, and biointerfaces. Here, we demonstrate that multi-layer graphene (MLG), like single-layer graphene (SLG), can self-fold to form 3D architectures at the interface with a polymeric film. Bilayers composed of graphene and polymeric film tightly adhere to each other and possess a sloped internal strain, which leads to spontaneous rolling to predetermined 3D microscale architectures. The curvature radii of self-folding films can be controlled by changing the thicknesses of the polymeric film and the stacking order. In contrast to single-layer graphene, multilayer graphene shows no strain in most of the outer graphene layers and linear ohmic current characteristics after self-folding. Throughout the self-folding process, the conductance of MLG decreases but remains higher than that of SLG. This versatile way of forming a 3D multi-layer graphene structure is potentially applicable for fabrication of practical carbon devices without the changes in their conductive properties. (C) 2022 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).