The　reduction　of　nitrobenzene　(Ph-NO2)　to　aniline　(Ph-NH2)　utilizes　H2S　as　a　hydrogen　donor.　This　approach　alleviates　environmental　pollution　while　enabling　resource　utilization.　However,　it　remains　a　challenge　to　develop　sulfur-resistant　catalysts.　Herein,　we　fabricated　a　series　of　MoS2/ZrO2　catalysts　via　crystalline　phase　modulation　engineering　for　the　reduction　of　Ph-NO2　by　H2S　to　Ph-NH2.　Systematic　experiments　demonstrate　that　amorphous　ZrO2　has　the　highest　concentration　of　oxygen　vacancies　(Ov),　which　exhibits　the　highest　activity　and　stability.　As　a　result,　the　MoS2/a-ZrO2　achieves　a　Ph-NO2　conversion　of　92　%　and　a　Ph-NH2　selectivity　of　85.7　%　at　1.5　MPa　and　90　°C,　which　is　superior　to　MoS2/m-ZrO2,　MoS2/t-ZrO2,　MoS2　and　ZrO2.　In　situ　FT-IR　measurements　combined　with　full　two-dimensional　time　of　flight　chromatography　suggest　a　double　H-induced　dissociation　pathway　for　the　reduction　of　Ph-NO2　to　Ph-NH2　by　H2S.　This　study　offers　a　viable　strategy　for　the　valorization　of　H2S　into　valuable　resources.　©　2025　Hydrogen　Energy　Publications　LLC