The controlled etching of 2D transition metal dichalcogenides (2D‐TMDs) is critical to understanding the growth mechanisms of 2D materials and patterning 2D materials but remains a major comprehensive challenge. Here, a rational strategy to control the terminal atoms of 2D‐TMDs etched holes is reported. Using laser irradiation combined with an improved anisotropic thermal etching process under a determined atmosphere, terminal atom‐controlled etched hole arrays are created on 2D‐TMDs. By adjusting the gas atmosphere during the thermal etching stage, triangular etched hole arrays terminated by the tungsten zigzag (W‐ZZ) edge (in an Ar/H2 atmosphere), hexagonal etched hole arrays terminated alternately by the W‐ZZ edge and sulfur (selenium) zigzag (S‐ZZ or Se‐ZZ) edge (in a pure Ar atmosphere), and triangular etched hole arrays terminated by the S‐ZZ (Se‐ZZ) edge (in an Ar/sulfur [selenium] vapor atmosphere) can be obtained. Density functional theory reveals the forming energy of different edges and the different activities of metal atoms and chalcogenide atoms under different atmospheres, which determine the terminal atoms of the holes. This work may enhance the understanding of the etching and growth of 2D‐TMDs. The 2D‐TMDs hole arrays constructed by this work may have important applications in catalysis, nonlinear optics, spintronics, and large‐scale integrated circuits.