This　work　shows　the　molecular　engineering　of　metal　active　sites　on　the　surface　of　anatase　nanoparticles,　based　on　the　fundamental　of　metal-to-metal　charge　transfer　(MMCT).　A　series　of　Sn,　Ni-co-modified　TiO2　photocatalysts　were　prepared　by　use　of　surface　organometallic　chemistry.　Photocatalytic　hydrogen　production　from　ethylenediaminetetraacetic　acid　disodium　salt　solution　as　a　model　reaction　was　used　to　evaluate　the　photocatalytic　properties　of　the　materials.　The　chemical　states　of　the　modifiers　were　characterized　by　a　combination　of　various　spectroscopic　techniques.　These　results　clearly　reveal　the　synergy　of　atomically　isolated　Ni　and　Sn　centers　for　solar-to-hydrogen　conversion.　A　near　10-fold　enhancement　of　hydrogen　production　is　achieved　on　Sn,　Ni-co-grafted　TiO2　photocatalysts　under　solar　light　irradiation.　Detailed　characterization　suggests　that　the　synergy　is　closely　related　to　the　[-O-Ti-O-Sn-O-Ni-O-Ti-]　heteroatomic　clusters　with　the　eight-member　cyclic　structure.　An　electron-delocalization　loop　is　proposed　for　efficient　separation　of　charges　photogenerated　in　bulk　TiO2　and　excitons　generated　in　Ni-O-Ti　molecular　linkages.