Interface-driven multifunctional facets are gearing up in the field of science and technology. Here, we present the interface-activated resistive switching (RS), negative differential resistance, diode behavior, and ultraviolet (UV) light sensing in nanosheet-based hybrid devices. A hybrid device i.e., titanium dioxide nanosheet (TiO 2 -NS)/poly(dimercaptothiadiazoletriazine)[Poly(DMcT-CC)] is fabricated by spin coating Poly-(DMcT-CC) polymer on hydrothermally as-grown TiO 2 -NS. The pristine devices of both materials show either small or no magnitude of RS, but the hybrid device shows highly enhanced RS of nearly four orders due to the formation of a p−n junction at the NS/polymer interface. The resistive random access memory feature appears to be more prominent in the hybrid device i.e., high and low current states are found to be stable in repetitive cycles since the interface acts as a trapping center for the carriers. The UV sensing ability of the hybrid device has been demonstrated by a threefold increment in a current at 60 mV. The impedance spectroscopy has been employed to show that the multifunctional features are directly associated to the NS/polymer interface, which deduce that the manipulation of such interfaces can pave the way for developing the hybrid structures.