The employment of single atoms (SAs), especially Pt SAs, as co‐catalysts in photocatalytic H2 generation has gained significant attention due to their exceptional efficiency. However, a major challenge in their application is the light‐induced agglomeration of these SAs into less active nanosized particles under photocatalytic conditions. This study addresses the stability and reactivity of Pt SAs on TiO2 surfaces by investigating various post‐deposition annealing treatments in air, Ar, and Ar‐H2 environments at different temperatures. We describe that annealing in an Ar‐H2 atmosphere optimally stabilizes SA configurations, forming stable 2D rafts of assembled SAs approximately 0.5‐1 nm in diameter. These rafts not only resist light‐induced agglomeration but also exhibit significantly enhanced H2 production efficiency. Our findings reveal a promising approach to maintaining the high reactivity of Pt SAs while overcoming the critical challenge of their stability under photocatalytic conditions.This article is protected by copyright. All rights reserved