A series of dual-band photomultiplication (PM)-type organic photodetectors (OPDs) were fabricated by employing a donor(s)/acceptor (100:1, wt/wt) mixed layer and an ultrathin Y6 layer as the active layers, as well as by using PNDIT-F3N as an interfacial layer near the indium tin oxide (ITO) electrode. The dual-band PM-type OPDs exhibit the response range of 330−650 nm under forward bias and the response range of 650−850 nm under reverse bias. The tunable spectral response range of dual-band PM-type OPDs under forward or reverse bias can be explained well from the trapped electron distribution near the electrodes. The dark current density (J D ) of the dual-band PM-type OPDs can be efficiently suppressed by employing PNDIT-F3N as the anode interfacial layer and the special active layers with hole-only transport characteristics. The light current density (J L ) of the dualband PM-type OPDs can be slightly increased by incorporating wide-bandgap polymer P-TPDs with relatively large hole mobility (μ h ) in the active layers. The signal-to-noise ratios of the optimized dual-band PM-type OPDs reach 100,980 under −50 V bias and white light illumination with an intensity of 1.0 mW•cm −2 , benefiting from the ultralow J D by employing wide-bandgap PNDIT-F3N as the anode interfacial buffer layer and the increased J L by incorporating appropriate P-TPD in the active layers.