In this study, we investigate the bulk effect of photoresponsive gate insulators on the photoresponse of organic phototransistors (OPTs), using OPTs with poly(4-vinylphenol) layers of two different thicknesses. For the photoresponse, the interplay between the charge accumulation (capacitance) and light-absorbance capabilities of a photoresponsive gate insulator was investigated. Although an OPT with a thicker gate insulator exhibits a lower capacitance and hence a lower accumulation capability of photogenerating charges, a thicker poly(4-vinylphenol) layer, in contrast to a thinner one, absorbs more photons to generate more electron–hole pairs, resulting in a higher photoresponse of the device. That is, in these two cases, the degree of light absorption by the photoresponsive gate insulators dominantly governed the photoresponse of the device. Our physical description of the bulk effect of photoresponsive insulators on the performance of OPTs will provide a useful guideline for designing and constructing high-performance organic-based photosensing devices and systems.