Carbon　quantum　dots　(CQDs)　have　recently　emerged　as　the　light-harvesting　antennas　for　photocatalytic　applications　due　to　their　outstanding　optical　absorption,　nontoxicity,　unsophisticated　synthesis　and　scalable　production.　However,　the　poor　photocatalytic　efficiency　and　difficult　recovery　of　CQDs　restrict　their　large-scale　practical　applications　in　aqueous　photocatalytic　reactions.　Here　we　report　a　facile　synthesis　of　metal-free　three-dimensional　(3D)　construction　of　CQDs　spatially　distributed　into　the　frameworks　of　graphene　aerogel　(CQDs/GA)　with　enhanced　photocatalytic　performance　compared　to　the　bare　CQDs.　The　photoelectrochemical　characterizations　demonstrate　that　3D　graphene　aerogel　(GA)　with　interconnected　networks　exhibits　efficient　spatial　separation　and　transportation　of　photoexcited　charge　carriers,　thereby　leading　to　the　improved　photocatalytic　activity　of　the　CQDs/GA　composites.　In　addition,　such　3D　bulk　aerogel　displays　easy　separability　from　liquid　phase　reaction　system　and　regenerability　via　simple　replenishment　of　CQDs,　which　ensures　the　sustainable　photoactivity　of　the　CQDs/GA　composites.　This　approach　for　preparing　3D　CQDs/GA　composites　is　expected　to　open　a　new　vista　for　constructing　metal-free　and　regenerable　photocatalysts　with　enhanced　photosensitization　efficiency　of　CQDs.