Transition metal dichalcogenides (TMDs) are of interest for next‐generation electronics and optoelectronics owing to their unique optical and electronic functionalities. Although atomically thin flat TMD layers have been investigated in various device applications, pattern‐mediated growth serves great promise for revealing novel properties and application opportunities of TMDs. Herein, controlled size distribution of CVD‐grown monolayer MoS2 flakes by varying the distance between surface pattern features and the effects of patterning on the optical properties of MoS2 domains is reported. Larger flakes and higher uniformity in size distribution are obtained via patterning in comparison with the results from bare surface. Superior photoluminescence (PL) performances are observed for the 2D MoS2 grown on the pattern valleys when compared with the sample on the hill regions and the bare surface. The results demonstrate the notable potential of 2D TMDs for applications in electronics and optoelectronics.

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