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Zero-valent copper (Cu0) is a promising co-catalyst in semiconductor-based photocatalysis as it is inexpensive and exhibits electronic properties similar to those of Ag and Au. However, its practical application in photocatalytic hydrogen production is limited by its susceptibility to oxidation, forming less active Cu species. Herein, we have carried out in situencapsulation of Cu0nanoparticles with N-graphitic carbon layers (14.4% N) to stabilize Cu0nanoparticles (N/C-coated Cu) and improve the electronic communication with a TiO2photocatalyst. A facile solvothermal procedure is used to coat the Cu0nanoparticles at 200 °C, while graphitization is achieved by calcination at 550 °C under an inert atmosphere. The resultant N/C-coated Cu/TiO2composites outperform the uncoated Cu counterparts, exhibiting a 27-fold enhancement of the hydrogen evolution rate compared to TiO2and achieving a rate of 19.03 mmol g–1h–1under UV–vis irradiation. Likewise, the N/C-coated Cu co-catalyst exhibits a less negative onset potential of −0.05 V toward hydrogen evolution compared to uncoated Cu (ca. −0.30 V). This superior activity is attributed to coating Cu0with N/C, which enhances the stability, electronic communication with TiO2, conductivity, and interfacial charge transfer processes. The reported synthetic approach is simple and scalable, yielding an efficient and affordable Cu0co-catalyst for TiO2.