Three　classical　Fe-MOFs,　viz.,　MIL-100(Fe),　MIL-101(Fe),　and　MIL-53(Fe),　were　synthesized　to　serve　as　platforms　for　the　investigation　of　structure-activity　relationship　and　catalytic　mechanism　in　the　selective　conversion　of　H2S　to　sulfur.　The　physicochemical　properties　of　the　Fe-MOFs　were　characterized　by　various　techniques.　It　was　disclosed　that　the　desulfurization　performances　of　Fe-MOFs　with　well-defined　microstructures　are　obviously　different.　Among　these,　MIL-100(Fe)　exhibits　the　highest　catalytic　performance　(ca.　100%　H2S　conversion　and　100%　S　selectivity　at　100-180　degrees　C)　that　is　superior　to　that　of　commercial　Fe2O3.　Furthermore,　the　results　of　systematic　characterization　and　DFT　calculation　reveal　that　the　difference　in　catalytic　performance　is　mainly　because　of　discrepancy　in　the　amount　of　Lewis　acid　sites.　A　plausible　catalytic　mechanism　has　been　proposed　for　H2S　selective　conversion　over　Fe-MOFs.　This　work　provides　critical　insights　that　are　helpful　for　rational　design　of　desulfurization　catalysts.