Selenium (Se)-rich binary Cu-Se and In-Se nanoparticles (NPs) were synthesized by a modified heat-up method at low temperature (110 °C) using the gum exudates from a cherry blossom tree. Coating of CISe absorber layer was carried out using Se-rich binary Cu-Se and In-Se NPs ink without the use of any external binder. Our results indicated that the gum used in the synthesis played beneficial roles such as reducing and capping agent. In addition, the gum also served as a natural binder in the coating of CISe absorber layer. The CISe absorber layer was integrated into the solar cell, which showed a power conversion efficiency (PCE) of 0.37%. The possible reasons for low PCE of the present solar cells and the steps needed for further improvement of PCE were discussed. Although the obtained PCE is low, the present strategy opens a new path for the fabrication of eco-friendly CISe NPs solar cell by a relatively chief non-vacuum method.