Because of its thickness‐dependent direct bandgap and exceptional optoelectronic properties, indium(III) selenide (In2Se3) has emerged as an important semiconductor for electronics and optoelectronics. However, the scalable synthesis of defect‐free In2Se3 flakes remains a significant barrier for its practical applications. Here, a facile electrochemical strategy is presented for the ultrafast delamination of bulk layered In2Se3 crystals in nonaqueous media, resulting in high‐yield (83%) production of defect‐free In2Se3 flakes with large lateral size (up to 26 µm). The intercalation of tetrahexylammonium (THA+) ions mainly creates stage‐3 intercalated compounds in which every three layers of In2Se3 are occupied by one layer of THA molecules. The subsequent exfoliation leads to a majority of trilayer In2Se3 nanosheets. As a proof of concept, solution‐processed, large‐area (400 µm × 20 µm) thin‐film photodetectors embedded with the exfoliated In2Se3 flakes reveal ultrafast response time with a rise and decay of 41 and 39 ms, respectively, and efficient responsivity (1 mA W−1). Such performance surpasses most of the state‐of‐the‐art thin‐film photodetectors based on transition metal dichalcogenides.