Abstract The band gap of few‐layered 2D material is one of the significant issues for the application of practical devices. Due to the outstanding electrical transport property and excellent photoresponse, 2D InSe has recently attracted rising attention. Herein, few‐layered InSe nanosheets with direct band gap are delivered by a facile liquid‐phase exfoliation approach. We have synthesized a photoelectrochemical (PEC)‐type few‐layered InSe photodetector that exhibits high photocurrent density, responsivity, and stable cycling ability in KOH solution under the irradiation of sunlight. The detective ability of such PEC InSe photodetector can be conveniently tuned by varying the concentration of KOH and applied potential suggesting that the present device can be a fitting candidate as an excellent photodetector. Moreover, extendable optimization of the photodetection performance on InSe nanosheets would further enhance the potential of the prepared InSe in other PEC‐type devices such as dye‐sensitized solar cells, water splitting systems, and solar tracking equipment.

High‐Performance Photo‐Electrochemical Photodetector Based on Liquid‐Exfoliated Few‐Layered InSe Nanosheets with Enhanced Stability