The successive ionic layer adsorption and reaction (SILAR) method was used to deposit several CdSe quantum dots (QDs) on the surface of g-C 3 N 4 nanosheets. In comparison to the single moiety of g-C 3 N 4 , as-prepared heterostructures displayed an improved bifunctional photo-and electrocatalytic activity for oxygen (OER) and hydrogen evolution reactions (HER). Significantly, the 30 SILAR cycles optimized CdSe QDs/g-C 3 N 4 heterostructure exhibited high performances and stabilities for the OER and HER reaction in alkaline conditions. The as-prepared heterostructure catalyst also exhibited an efficient photocatalytic activity toward the H 2 evolution reaction and produced 4306 μmol of H 2 gas with 23.8% of apparent quantum yield in the presence of triethanolamine as a sacrificial agent. Photoluminescence spectroscopy, electron paramagnetic resonance, and impedance spectroscopy suggest that the synergy between g-C 3 N 4 nanosheets and CdSe QDs leads to higher catalytic activities, as indicated by the low overpotentials of 147 and 218 mV to obtain a 10 mA cm −2 current density for the HER and OER reactions, respectively. Furthermore, in situ Fourier transform infrared spectroscopy, liquid chromatography−mass spectroscopy, and high-performance liquid chromatography were conducted to determine the photochemical intermediate products to confirm the successful oxidation of TEOA by capturing holes. The outcome is in accordance with the fact that the photogenerated electrons are transferred from the conduction band (CB) of g-C 3 N 4 nanosheets to the valence band (VB) of CdSe QDs in a Z-scheme manner.