Photomultiplication (PM) structure has been widely employed to improve the optoelectronic performance of organic photodetectors (OPDs). However, most PM-type OPDs require a high negative operating voltage or complex fabrication. For obtaining high-efficiency OPDs with low voltage and easy process, here the bulk heterojunction (BHJ) structure of high exciton dissociation efficiency combined with the method of trap-assisted PM are applied to the OPDs. In this paper, we investigate the operating mechanism of OPDs based on poly(3-hexylthiophene) (P3HT): (phenyl-C61butyric-acid-methyl-ester) (PC 61 BM), and poly-{ [4,8-bis[(2-ethylhexyl) [3,4-b]thiophene-4,6-diyl]} (PBDT-TT-F):PC 61 BM doped with C 60 as active layer. Furthermore, the influence of C 60 concentration on the optoelectronic performances is also discussed. With 1.6 wt.% C 60 added, the P3HT:PC 61 BM:C 60 OPD exhibits a 327.5% external quantum efficiency, a 1.21 A•W −1 responsivity, and a 4.22 × 10 12 Jones normalized detectivity at −1 V under 460 nm (0.21 mW•cm −2 ) illumination. The experimental results show that the effective electron traps can be formed by doping a small weight of C 60 into BHJ active layer. Thus the PM-type OPDs can be realized, which benefits from the cathode hole tunneling injection assisted by the trapped electrons in C 60 near the Al side. The efficiency of PM is related to the C 60 concentration. The present study provides theoretical basis and method for the design of highly sensitive OPDs with low operating voltage and facile fabrication.