AbstractThe interference of electronic wavefunctions within a Kagome lattice can result in a flat band structure, where low‐energy electrons exhibit highly correlated behavior, facilitating exploration of interactions among intriguing electronic states. However, the inherent high carrier density in most known Kagome materials often hampers the manipulation of these quantum phenomena through conventional means, such as gate voltage. In this work, a unique tunability in the electrical and optoelectronic properties of exfoliated Nb3I8, a 2D semiconductor featuring a “breathing” Kagome lattice is uncovered. Characterization via temperature‐dependent ARPES confirms its semiconducting nature with a flat band structure. Experimental results from bias and gate voltage dependent transport measurements on thin film Nb3I8 transistor devices demonstrate ambipolar conductance. Notably, these findings reveal a broadband photoresponse in the device, spanning from visible to near infrared wavelengths (532 −1100 nm), with the photocurrent showing gate‐dependent characteristics that mirror the dark current's ambipolar nature. This observation marks the first instance of ambipolar transport in a Kagome semiconductor, opening up exciting new avenues for electronic and optoelectronic device development.