We demonstrate an approach to enhancing the photoresponsivity of a polymer photodetector (PPD). Both conventional bulk heterojunction (BHJ) and planar heterojunction (PHJ) PPDs were fabricated considering that the interface between a CdSe nanocrystal and a polymer can create photoconductive gain. A systematic study of the illumination wavelength and light power dependence of the photocurrent gain, combined with the charge carrier transport analysis, suggested that the PHJ-PPD could yield a higher hole mobility than could be achieved in a BHJ-PPD without compromising on the selective electron trapping effects. The optimized PHJ-PPD led to a photoconductive detectivity of 1.3 × 1010 cm Hz1/2/W.