Here, we demonstrated the quantum heterojunction colloidal quantum dot (CQD) solar cells employing the PbS CQDs/Cd3P2 CQDs architecture in which both the p-type PbS and n-type Cd3P2 CQD layers are quantum-tunable and solution-processed light absorbers. We synthesized well-crystallized and nearly monodispersed tetragonal Cd3P2 CQDs and then engineered their energy band alignment with the p-type PbS by tuning the dot size and hence the bandgap to achieve efficient light absorbing and charge separation. We further optimized the device through the Ag-doping strategy of PbS CQDs that may leverage an expanded depletion region in the n-layer, which greatly enhances the photocurrent. The resulting devices showed an efficiency of 1.5%.