Wafer‐Scale Ultrafine Wrinkle Architectures of TMDCs for Multifunctionality

Intensely applied strain from wrinkled architecture mitigates intrinsic limitations of 2D materials while enhancing their capabilities through spatially modulated electronic and catalytic properties. Here, this study introduces a deterministic wafer‐scale fabrication strategy that enables densely distributed ultrafine wrinkled architectures in atomically thin molybdenum disulfide (MoS 2 ) crystals, achieving tensile strains up to 3.29% over 50% of the scan area. The wrinkle structures are obtained by modulating the parameters of a wet transfer method, including transfer liquid media, thermal energy, and polystyrene (PS) solution concentrations. Collectively, these results demonstrate a practical route to wafer‐scale fabrication of ultrafine wrinkle structures. The wrinkled MoS 2 (w‐MoS 2 ) exhibits optimal multifunctional device performance in electronics and as a hydrogen evolution catalyst. In a hydrogen evolution reaction (HER), the lowest Tafel slope (52.3 mV dec −1 ) is observed, comparable to that of metallic TMDC catalysts. Furthermore, our w‐MoS 2 memory device displays an on/off ratio of 5 × 10 7 with a large memory window corresponding to 65% of the total gate voltage ( V GS ) sweep range. This simple and innovative morphology engineering offers a viable and reproducible pathway toward high‐performance electronic and catalytic functionalities in highly strained 2D materials.