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Increasing the efficiency of visible-light-driven water splitting systems will require improvements in the charge separation characteristics and redox reaction kinetics associated with narrow-bandgap photocatalysts. Although the traditional approach of loading a single cocatalyst on selective facets provides reaction sites and reduces the reaction overpotential, pronounced surface charge carrier recombination still results in limited efficiency increases. The present study demonstrates a significant improvement in the hydrogen evolution activity of the layered single-crystal photocatalyst Y 2 Ti 2 O 5 S 2 . Increased performance is obtained through sequential loading of Pt cocatalysts using a two-step process followed by photodeposition of Cr 2 O 3 nanolayers. The stepwise deposition of Pt involved an impregnation-reduction pretreatment with subsequent photodeposition and produced numerous hydrogen production sites while promoting electron capture. The Cr 2 O 3 shells formed on Pt nanoparticles further promoted electron transfer from the Pt to the water and inhibited surface carrier recombination. Importantly, it is also possible to construct a Z-scheme overall water splitting system using the optimized Y 2 Ti 2 O 5 S 2 in combination with surface-modified BiVO 4 in the presence of [Fe(CN) 6 ] 3-/4- , yielding a solar-to-hydrogen energy conversion efficiency of 0.19%. This work provides insights into precise surface modifications of narrow-bandgap photocatalysts as a means of improving the solar water splitting process., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)