Van der Waals (vdW) integration, in which pre-engineered two-dimensional building blocks are physically assembled together in a chosen sequence through weak vdW interactions, holds promise toward previously unattainable applications. However, when extended to create 3D/3D monoliths, the lack of physical bonding coupled with the inherent rigidity and surface roughness between 3D building blocks makes it challenging for broader implementation of composites, catalysis, and energy applications. Here we demonstrate that electrostatically exfoliated two-dimensional layered materials can be additively manufactured to create complex layouts with selectively engineered composition in both lateral and vertical directions. Subsequent room-temperature dewetting creates non-covalent hinges through folded edges to concurrently interlock and nanostructure the two-dimensional inks into 3D building blocks. The result is the 3D/3D vdW mono- and heterostructures that are mechanically robust, electrically conductive, electrochemically active over a broad pH range and even radiation tolerant in nature.

Van der Waals（vdW）集成（通过微弱的vdW交互以选定的顺序将预先设计的二维构建块物理组装在一起）对以前无法实现的应用程序具有希望。但是，当扩展为创建3D / 3D整体时，缺少物理键合以及3D构建块之间固有的刚性和表面粗糙度，这使其对复合材料的广泛实施，催化和能源应用提出了挑战。在这里，我们证明了静电剥落的二维层状材料可以通过增材制造来创建具有横向和垂直方向选择性成分的复杂布局。随后的室温去湿通过折叠的边缘创建非共价铰链，以同时将二维墨水互锁和纳米结构化为3D构建块。结果是3D / 3D vdW单结构和异结构在较宽的pH范围内具有机械坚固性，导电性，电化学活性，甚至具有耐辐射性。