Solar water splitting has emerged as an urgent imperative as hydrogen emerges as an increasingly important form of energy storage. g-C3N4 is an ideal candidate for photocatalytic water splitting as a result of the excellent alignment of its band edges with water redox potentials. To mitigate electron-hole recombination that has limited the performance of g-C3N4, we have developed a semiconductor heterostructure of g-C3N4 with CuFe2O4 nanoparticles (NPs) as a highly efficient photocatalyst. Visible-light-driven photocatalytic properties of CuFe2O4/g-C3N4 heterostructures with different CuFe2O4 loadings have been examined with two sacrificial agents. An up to 2.5-fold enhancement in catalytic efficiency is observed for CuFe2O4/g-C3N4 heterostructures over g-C3N4 nanosheets alone with the apparent quantum yield of H2 production approaching 25%. The improved photocatalytic activity of the heterostructures suggests that introducing CuFe2O4 NPs provides more active sites and reduces electron-hole recombination. The g-C3N4/CuFe2O4 heterostructures furthermore show enhanced electrocatalytic HER activity as compared to the individual components as a result of which by making heterostructures g-C3N4 with CuFe2O4 increased the active catalytic surface for the electrocatalytic water splitting reaction. The enhanced faradaic efficiency of the prepared heterostructures makes it a potential candidate for efficient hydrogen generation. Nevertheless, the designed heterostructure materials exhibited significant photo- and electrocatalytic activity toward the HER, which demonstrates a method for methodically enhancing catalytic performance by creating heterostructures with the best energetic offsets.