A simple method is developed through drop-casting techniques to assemble a molybdenum disulfide (MoS2)-reduced graphene oxide (rGO) hybrid on vertically aligned carbon nanotubes (VACNTs) to perform as an optoelectronic device for nitrogen dioxide (NO2) gas sensing at room temperature. The VACNT not only forms an ohmic contact with the hybrid material, but also yields a weak charge impurity scattering in the rGo layers across the channel. These features dramatically affect the optical response of the device to the light through which improve the photoresponsivity by up to 236% and the response time by up to 40% compared to the Au contacted device. Next, the fabricated MoS2-rGo/VACNTs device is employed as a resistor gas sensor for NO2 under in situ exposure to the light at room temperature. Under laser illumination, the sensor demonstrates a high sensitivity of ~ 41% at an inlet NO2 concentration of 100 ppm with a complete recovery time of ~150 s which shows comparable improvements relative to the sensor performance in dark condition.