Protonated g-C3N4 (pCN) formed by treating bulk g-C3N4 with an aqueous HCl solution was modified with D149 dye, i.e., 5-[[4[4-(2,2-diphenylethenyl) phenyl]-1,2,3,3a,4,8b-hexahydrocyclopent[b]indol-7-yl] methylene]-2-(3-ethyl-4-oxo-2-thioxo-5-thiazolidinylidene)-4-oxo-thiazolidin-2-ylidenerhodanine, for photocatalytic water splitting (using Pt as a co-catalyst). The D149/pCN-Pt composite showed a much higher rate (2138.2 µmol·h−1·g−1) of H2 production than pCN-Pt (657.0 µmol·h−1·g−1). Through relevant characterization, the significantly high activity of D149/pCN-Pt was linked to improved absorption of visible light, accelerated electron transfer, and more efficient separation of charge carriers. The presence of both D149 and Pt was found to be important for these factors. A mechanism was proposed.