Emerging Nonplanar van der Waals Nanoarchitectures from 2D Allotropes for Optoelectronics

The unique atomic thickness and mechanical flexibility of 2D van der Waals (vdW) materials endow them with spatial designability and constructability. It is easy to break the inherent planar construction through various spatial manipulations, thus creating vdW nanoarchitectures with nonplanar topologies. The basic properties before evolution are retained and tunable by architecture‐related feature sizes, and other newly generated properties are inspiring as they are beyond the reach of 2D allotropes, bringing great competitiveness for their encouraging applications in optoelectronics. Here, these representative nonplanar vdW nanoarchitectures (i.e., nanoscrolls, nanotubes, spiral nanopyramids, spiral nanowires, nanoshells, etc.) are summarized and their structural evolution processes are elucidated. Their fascinating nascent properties based on their distinctive structural features, focusing on generally enhanced light–matter interactions and device physics, are further introduced. Finally, their opportunities and challenges for in‐depth experimental exploration are prospected. It is a brand‐new idea to modify the properties of 2D vdW materials from micro‐ and nanostructural design and evolution, offering a solid platform for twistronics, valleytronics, and integrated nanophotonics. Structure–processing–property–performance paradigm of materials science provides key guidance for obtaining unprecedented nonplanar van der Waals (vdW) nanoarchitectures. In this review, critical summary and deep insights are provided on the recent development of these emerging nonplanar vdW nanoarchitectures, specifically, nanoscrolls, nanotubes, nanospirals, nanoshells, etc., with the aim to realize the practical optoelectronic applications at the nanoscale.