Influence on photocurrent sensitivity of hydrothermally synthesized electrochemically active graphene quantum dots on conjugated polymer utilized for a novel single-layer device has been performed. Fabrications of high-performance ultraviolet photodetector by depositing the polypyrrole-graphene quantum dots (PPy-GQDs) active layer of the ITO electrode were exposed to an Ultraviolet (UV) source with 265 and 355 nm wavelengths for about 200 s, and we examined the time-dependent photoresponse. The excellent performance of GQDs was exploited as a light absorber, acting as an electron donor to improve the carrier concentration. PGC4 exhibits high photoresponsivity up to the 2.33 µA/W at 6 V bias and the photocurrent changes from 2.9 to 18 µA. The electrochemical measurement was studied using an electrochemical workstation. The cyclic voltammetry (CV) results show that the hysteresis loop is optically tunable with a UV light source with 265 and 355 nm at 0.1 to 0.5 V/s. The photocurrent response in PPy-GQDs devices may be applicable to optoelectronics devices.