To　realize　highly　efficient　production　of　H2　and　conversion　of　biomass-relevant　alcohols　are　hot　spots　in　energy　and　environmental　science.　Herein,　we　have　fabricated　noble　metal-free　2D/2D-3D　NiS/Zn3In2S6　hierarchical　architecture　by　one-step　method　for　efficiently　visible-light-driven　dehydrogenation　of　5-hydroxymethylfurfural　(HMF)　into　H-2　and　2,5-diformylfuran　(DFF)　with　high　selectivity.　The　separation　of　photoexcited　electrons　(e(-))　and　holes　(h(+))　can　be　promoted　in　this　dual-function　photocatalysis　process.　More　importantly,　both　e(-)　and　h(+)　are　involved　in　the　desired　conversions,　i.e.　the　generation　of　H-2　and　the　production　of　value-added　chemicals,　respectively.　The　conversion　was　favored　not　only　by　thermodynamics,　but　also　kinetics.　The　H-2-evolution　rate　in　HMF　solution　was　up　to　1090.9　times　than　in　water.　Additionally,　the　DFF　selectivity　could　reach　up　to　94.1　%.　Such　designed　dual-function　photocatalytic　system　could　be　more　feasible　and　practical　in　the　perspective　of　the　sustainable　and　green　development.