Recent　years　have　witnessed　an　explosive　investigation　on　the　construction　of　graphene　(GR)-semiconductor　composite　photocatalysts,　but　the　specific　correlation　of　the　interface　integration　mode　between　GR　and　a　semiconductor　with　the　interfacial　charge　transfer　characteristics　is　yet　to　be　clearly　clarified.　To　this　end,　a　facile,　green　and　surface　linker-triggered　self-assembly　has　been　designed　to　construct　GR-encapsulated　antimony　sulfide　nanorod　(Sb2S3　NRs-GR)　ensembles,　wherein　tartaric　acid-capped　intrinsically　negatively　charged　Sb2S3　NRs　and　surface-modified　positively　charged　GR　nanosheets　were　utilized　as　the　building　blocks.　It　was　unveiled　that　the　exquisitely　designed　interface　configuration　afforded　by　the　intimate　encapsulation　of　Sb2S3　NRs　with　GR　via　an　electrostatic/hydrogen　interaction　is　beneficial　for　fully　harnessing　the　structural　merits　of　GR　in　boosting　light　absorption,　increasing　the　specific　surface　area　and　accelerating　the　interfacial　electron　transfer　kinetics.　Thus,　the　lifetimes　of　the　photogenerated　charge　carriers　were　synergistically　prolonged　over　Sb2S3,　resulting　in　the　considerably　enhanced　visible-light-responsive　photoredox　performances　of　the　Sb2S3-GR　nanocomposites　toward　the　photoreduction　of　heavy　metal　ions　and　mineralization　of　organic　pollutants　compared　with　the　blank　Sb2S3　and　nanocomposite　counterpart　without　a　finely　tuned　interface.　More　importantly,　the　crucial　role　of　interface　configuration　between　GR　and　the　Sb2S3　NRs　in　dictating　the　interfacial　charge　transfer　efficiency　was　substantiated.　In　addition,　the　predominant　active　species　in　the　photoredox　catalysis　were　determined　and　the　corresponding　photocatalytic　mechanism　was　elucidated.　Our　work　sheds　light　on　mediating　the　interfacial　charge　transfer　via　rational　interface　configuration　modulation　toward　substantial　solar　energy　conversion.