Ultralarge　graphene-based　TiO2　nanosheet　composites　are　successfully　fabricated　by　a　noncovalent　functionalization　approach　with　use　of　benzyl　alcohol　as　the　linking　agent.　In　the　synthetic　procedure,　the　aromatic　molecules　of　benzyl　alcohol　direct　themselves　onto　graphene　(GR)　surface　via　π-π　interaction.　Therefore,　the　basal　planes　of　GR　nanosheets　are　uniformly　functionalized　with　hydroxyl　groups　derived　from　benzyl　alcohol,　which　not　only　improves　the　dispersion　of　GR　in　solution　but　also　induces　a　finely　homogeneous　coating　of　TiO2　nanocrystals　onto　the　surface　of　GR　nanosheets.　The　resulting　GR@TiO2　nanocomposites,　which　feature　unique　ultralarge　2D　sheet-like　morphology　with　the　lateral　size　far　larger　than　the　original　GR　and　densely　interfacial　contact,　are　able　to　act　as　highly　active　photocatalysts　toward　selective　reduction　of　aromatic　nitro　compounds　to　amines　in　water　under　ambient　conditions.　The　higher　photoactivity　of　GR@TiO2　than　blank　TiO2　is　attributed　to　the　efficient　charge　carriers　separation　and　transfer　by　the　GR　platform.　It　is　hoped　that　the　facile　synthesis　strategy　in　this　work　could　contribute　to　fabricating　other　ultralarge　functional　GR-based　2D　sheet-onto-sheet　composites　with　tunable　morphology　toward　target　photocatalytic　applications.　(Figure　Presented).　©　2014　American　Chemical　Society.