Photocatalytic　chemical　transformations　for　green　organic　synthesis　has　attracted　much　interest.　However,　their　development　is　greatly　hampered　by　the　lack　of　sufficient　reactive　sites　on　the　photocatalyst　surface　for　the　adsorption　and　activation　of　substrate　molecules.　Herein,　we　demonstrate　that　the　introduction　of　well-defined　Lewis　and　Brønsted　acid　sites　coexisting　on　the　surface　of　TiO2　(SO42−/N-TiO2)　creates　abundant　active　adsorption　sites　for　photoredox　reactions.　The　electron-deficient　Lewis　acid　sites　supply　coordinatively　unsaturated　surface　sites　to　adsorb　molecular　oxygen,　and　the　Brønsted　acid　sites　are　liable　to　donate　protons　to　form　hydrogen　bonds　with　the　OH　groups　of　alcohols　like　benzyl　alcohol　(BA).　These　coexistent　acid　sites　result　in　a　strong　synergistic　effect　in　photocatalytic　aerobic　oxidation　of　BA.　For　example,　the　conversion　of　BA　to　benzaldehyde　was　found　to　be　88.6　%,　being　much　higher　than　those　of　pristine　TiO2　(14.7　%),　N-doped　TiO2　(N-TiO2,　24.6　%),　sulfated　TiO2　(SO42−/　TiO2,　35.4　%),　and　even　their　sum.　The　apparent　quantum　efficiency　(AQE)　was　determined　to　be　58.1　%　at　365　nm　and　12.9　%　at　420　nm　over　SO42−/N-TiO2.　This　strategy　to　create　effective　synergistic　Lewis　and　Brønsted　acids　on　the　catalyst　surfaces　enables　us　to　apply　it　to　other　semiconducting　photocatalytic　organic　transformations.　©　2025　Wiley-VCH　GmbH.