Abstract2D Transition Metal Dichalcogenides hold a promising potential in future optoelectronic applications due to their high photoresponsivity and tunable band structure for broadband photodetection. In imaging applications, the detection of weak light signals is crucial for creating a better contrast between bright and dark pixels in order to achieve high resolution images. The photogating effect has been previously shown to offer high light sensitivities; however, the key features required to create this as a dominating photoresponse has yet to be discussed. Here, we report high responsivity and high photogain MoS2 phototransistors based on the dual function of HfO2 as a dielectric and charge trapping layer to enhance the photogating effect. As a result, these devices offered a very large responsivity of 1.1 × 106 A W−1, a photogain >109, and a detectivity of 5.6 × 1013 Jones under low light illumination. This work offers a CMOS compatible process and technique to develop highly photosensitive phototransistors for future low-powered imaging applications.