Self-powered photodetectors with bipolar photoresponse characteristics are expected to play a critical role in the field of secure optical communication, artificial neuromorphic systems, and intelligent color sensors. In this work, asymmetric heterojunction devices exhibiting wavelength-dependent bipolar photoresponse with a structure of Glass/FTO/CdSe/Bi 2 Se 3 /Au were fabricated. Under a short wavelength light irradiation, the top CdSe absorber generates a high carrier concentration; the excited carriers are quickly separated by the built-in electric field induced by the FTO/CdSe diode, resulting in a negative photocurrent. For light with wavelengths beyond the CdSe absorption edge, it is absorbed by the bottom Bi 2 Se 3 absorber, and a positive photocurrent can be observed. Therefore, based on the bandgap difference between the top CdSe absorber and the bottom Bi 2 Se 3 absorber, combined with the photogenerated carriers separated by asymmetric back-toback diode, a wavelength-dependent bipolar response is realized. In this work, by employing this structure, the responsivities of −33.3 and 0.3 mA/W were achieved under the illumination of 405 and 830 nm, respectively. This work provides important indications in the preparation and performance optimization for wavelength-dependent bipolar photodetectors.