Bimetallic　alloy　AuPt　nanoclusters　supported　on　monolayer　H1.07Ti1.73O4·H2O　nanosheets　(AuPt/TN)　jointly　complete　a　rapid　catalytic　reaction　toward　hydrogenation　of　halonitrobenzene　to　haloaniline　in　methanol　under　ambient　conditions　using　HCOONH4　as　a　hydrogen　source.　Especially,　AuPt/TN　with　a　Au/Pt　molar　ratio　of　1:2　exhibits　the　high　catalytic　conversion　efficiency　for　halonitrobenzene　(＞99%)　with　a　high　selectivity　of　haloaniline　(＞99%).　In　situ　FTIR　spectra　suggest　that　the　TN　affords　surface　Brønsted　acid　sites　to　chemisorb　and　activate　the　halonitrobenzene　molecules　via　the　surface　hydrogen　bond　coordination.　In　situ　ESR　experiments　indicate　that　HCOONH4　would　be　decomposed　to　H+　and　a　•CO2-　radical　by　photogenerated　holes,　serving　as　the　hydrogen　source　and　reducing　species　for　the　reduction　of　the　-NO2　group,　respectively.　Experimental　results　reveal　that　atom　Pt　in　alloy　is　responsible　for　the　hydrogenation,　while　Au　represses　the　dehalogenation　of　haloanilines.　Finally,　a　possible　synergetic　mechanism　is　discussed.　This　work　highlights　that　the　multifunctional　AuPt/TN　catalyst　with　multiple　active　sites　exerts　the　respective　functions　to　cooperatively　catalyze　organic　transformations　toward　desired　target　products.　Copyright　©　2018　American　Chemical　Society.