Single atom (SA) catalysis, over the last 10 years, has become a forefront in heterogeneous catalysis, electrocatalysis, and most recently also in photocatalysis. Pt SAs on titania have been reported to be a highly effective co-catalyst in photocatalytic H2 generation. Most recently, for the synthesis of SA loading on titania surfaces, some simple immersion techniques have been described. Here we introduce a so far unexplored but evidently very effective approach to enhance the effectivity of Pt SA co-catalysts on anodic TiO2 layers. For this, we first decorate TiO2 surfaces with a partial coverage of headgroups of silane self-assembled monolayers (SAMs) and then deposit Pt SAs on this SAM modified surface. We observe a significantly enhanced photocatalytic activity for H2 generation using this sensitization of the surface with a modified SAM.