Wafer-scale 2D materials: from single-crystalline epitaxy to artificial stacking

Abstract Two-dimensional van der Waals (vdW) materials constitute a unique class of layered crystals in which adjacent layers are bonded through weak vdW interactions. Their orientation, stacking sequence, and twist angle can be precisely engineered, enabling atomic-level modulation of electronic structures and interfacial properties. This structural tunability has led to the discovery of diverse emergent phenomena in stacking, twisting, and heterointegration. Yet most of these findings rely on atomically defined local configurations, and extending such deterministic arrangements to wafer-scale level remains a central challenge for practical implementation. Recent years have witnessed major progress in the wafer-scale growth of single-crystalline vdW materials. Advances in symmetry-guided epitaxy, step-edge mediation, and interfacial engineering have elucidated how orientational selection, nucleation barriers, and seamless coalescence arise from substrate–film coupling. Meanwhile, stacking and twisting technologies have made notable progress in scalability and interfacial cleanliness, now enabling the assembly of large-area, deterministic vdW architectures. This Review provides a unified overview of the growth and stacking strategies that enable scalable deterministic atomic arrangements in vdW materials. Emphasis is placed on the correlations between structural configuration, interfacial characteristics, and functional performance in both homostructure stacking and lateral or vertical heterostructure fabrication. Finally, we highlight emerging directions—low-temperature epitaxy on non-epitaxial substrates, deterministic twist control for wafer-scale uniformity, and metrology connecting atomic order to device performance—toward rationally engineered, large-area vdW architectures.