electrical and optical characteristics, a large specific surface area, and great mechanical strength garnering a lot of interest in the field of high-performance and flexible optoelectronic devices. [3][4][5] 2D materials cover the spectrum from ultraviolet to terahertz (THz) waves and therefore most preferred materials for visible and THz optoelectronics. [6] Chemical doping and band engineering can alter the mid-infrared absorption of 2D materials. [7] 2D materials based photodetectors have been reported to exhibit suitable performance in the framework of plasma self-mixing and thermoelectric effect. [8,9] Graphene is a popular 2D material in broadband photo detectors because of its high carrier mobility. Limitations including lack of bandgap and weak optical absorption which restrict the production of photoexcited charge carries lead to low photoresponsity of ≈10 −1 A W −1 . [10][11][12] Modifying graphene properties have constrained its substantial utilization in photodetectors.Beyond graphene, 2D TMDCs is the group of van der Waals materials with a vast spectrum of electronic properties including metal-semimetal, semiconductor, and topological insulators due to diversity of structural phase and combination of transition metal and chalcogen atoms. [13] Some remarkable features of TMDCs such as direct bandgap, moderate in-plane mobility, low dark current and strong absorption in the visible region, and reasonable cost make them the most advanced materials for photonics and Few layered transition metal dichalcogenides (TMDCs) are widely used in electrochemical systems due to their unique optical and electronic properties including applications over a large area. Despite the widespread use of 2D layered materials as active components of photoanode, electrochemical conversion studies of few-layered Tantalum diselenide (TaSe 2 ) are still negligible. In view of this, the TaSe 2 nanocrystals (NCs) are successfully synthesized by using the facile liquid-phase exfoliation (LPE) approach. Different physiochemical characterization confirms the inherent physical and optical properties of TaSe 2 NCs. The flexible self-powered photoelectrochemical (PEC) type photodetector based on TaSe 2 NCs achieves the highest photocurrent density (P ph ) of 20.8 µA cm −2 and photoresponsivity (R ph ) of 0.208 mA W −1 in 0.5 m KOH. TaSe 2 NCs demonstrate the excellent self-driven ability and also unveil decent response under applied bias potential in different concentration of KOH electrolyte. Moreover, the electrode shows excellent ON/OFF switching stability up to 1000 s even after the 1 month of storage in the air. Importantly, the photodetector retains the P ph of 15.8 µA cm −2 after 95 bending cycles of 120° angle, displaying the great flexibility of TaSe 2 NCs. This work demonstrates the potential of TaSe 2 NCs for their extended application in PEC-type devices and flexible electronics.