ZnTi-LDH　nanosheets　have　been　synthesized　as　photocatalysts　for　selective　oxidation　of　benzyl　alcohol　(BA)　to　benzaldehyde　(BAD)　under　visible　light　irradiation.　Based　on　UV-vis　DRS,　in-situ　FTIR　and　XPS　results,　it　was　revealed　that　BA　would　be　efficiently　chemisorbed　and　activated　on　ZnTi-LDH　forming　the　surface　coordination　species,　which　contributed　to　harvesting　visible　light　and　induced　the　photocatalytic　reaction.　The　ESR　spectra　suggested　that　oxygen　vacancies　would　be　produced　in　ZnTi-LDHs　after　the　adsorption　of　BA　molecules.　More　exposed　surface　OH　groups　would　induce　more　oxygen　vacancies,　which　would　serve　as　the　centers　for　capturing　photoelectrons　from　the　photoexcited　surface　coordination　species　and　act　as　active　sites　for　enhanced　O-2　adsorption　and　activation,　resulting　outstanding　photocatalytic　activity.　Finally,　a　possible　mechanism　was　proposed　to　illustrate　the　photocatalytic　process　which　mediated　by　surface　coordination　species　formed　by　the　interaction　between　ZnTi-LDH　and　BA.