From Design to Prototype: High‐Sensitivity Tri‐Mode Operation Photodetectors Based on 1T‐2H Hybrid MoS 2

films via electrochemical intercalation technique, which intrinsically integrates a 2H-phase photosensitive network with a 1T-phase dispersed capacitance. By modulating the external bias and phase distribution, a family of photodetectors with tailored tri-mode operation was achieved among reconfigured photocapacitive (PCC), photovoltaic (PV), photoconductive (PC) modes. Breaking the conventional perception of capacitors as parasitic components in optoelectronic devices, our work harnessed the capacitive effect as an effective signal source, enabling self-powered operation and high-sensitivity detection. It exhibits efficient charging pulses and superior self-resetting characteristics with a response speed reaching 19.2 ms and an average charge-discharge efficiency of 87.6%. From device design to application prototype, our proof-of-concept demonstrations in non-contact sensing, flame monitoring, and image reconstruction highlight the positive potential in intelligent sensing technologies. This study not only provides a novel design paradigm for phase engineering in multi-functional photodetection, but also its successful implementations hold significant promising for advancing intelligent optoelectronics, such as optoelectronic chips and biosensing.