In　this　work,　ZnTi-LDH　nanosheets　with　several　monolayer　thickness　were　prepared　as　photocatalysts　for　the　aerobic　oxidation　of　aniline　to　yield　nitrosobenzene　under　visible　light　irradiation.　UV-vis　DRS,　in　situ　FTIR　and　XPS　results　jointly　revealed　that　aniline　molecules　were　efficiently　chemisorbed　and　activated　on　ZnTi-LDH　to　form　surface　coordination　active　species,　improving　visible　light　absorption　and　inducing　the　photocatalytic　reaction.　The　surface　OH　groups　on　ZnTi-LDH　as　the　Bronsted　base　sites　facilitated　the　reductive　deprotonation　of　aniline　to　form　the　anilino　anion,　which　was　a　key　step　in　promoting　aniline　oxidation.　ESR　and　XPS　data　suggested　that　oxygen　vacancies　(OVs)　were　formed　due　to　the　interaction　between　exposed　OH　groups　and　aniline　molecules.　The　OVs,　as　the　centers　to　capture　photoelectrons,　achieve　the　reduction　of　oxygen　molecules　to　O-2(-)　radicals,　which　further　oxidize　anilino　species　to　produce　nitrosobenzene.　Finally,　a　possible　mechanism　was　proposed　to　reveal　the　photocatalytic　process　based　on　the　surface　coordination　activation　theory.