The responsivity (R) of a thin film photodetector is proportional to the product of its photo-induced carrier density (n) and mobility (μ). However, when choosing between layer heterojunction (LH) and bulk heterojunction (BH) field-effect phototransistors (FEpTs), it is still unclear which of the two device structures is more conducive to photodetection. A comparison study is performed on the two structures based on polymer and PbS quantum dot hybrids. Both devices exhibit ambipolar behavior, with μE ≈ μH = 3.7 cm2 V−1 s−1 for BH-FEpTs and μH = 36 cm2 V−1 s−1 and μE = 52 cm2 V−1 s−1 for LH-FEpTs. Because of the improvements in μ and the channel order degree (α), the responsivity of LH-FEpTs is as high as 101 A/W, which is as much as two orders of magnitude higher than that of BH-FEpTs (10−1A/W) under the same conditions. Although the large area of the BH improves both the exciton separation degree (β) and n in the BH-FEpT, the lack of an effective transport mechanism becomes the main constraint on high device responsivity. Therefore, LH-FEpTs are better candidates for use as photo detectors, and a “three-high” principle of high α, β, and μ is found to be required for high responsivity.