Efficient　removal　of　hydrogen　sulfide　(H2S)　is　significant　for　both　basic　catalytic　science　and　industrial　environmental　chemistry.　Herein,　a　novel　slurry　desulfurization　process　with　honeycomb-like　α-FeOOH@Fe-EDTA　as　a　desulfurizer　has　been　developed　for　the　removal　of　H2S.　The　slurry　reaction　process　is　appropriate　for　processing　H2S-polluted　gas　with　a　gas–liquid–solid　reactor　due　to　its　good　heat　transfer　and　diffusion　coefficient.　The　formation　of　Fe-EDTA　coordination　over　α-FeOOH@Fe-EDTA　effectively　enhanced　resistance　to　degradation　and　sulfation.　Importantly,　the　Fe3+/Fe2+　redox　mediator　endows　α-FeOOH@Fe-EDTA　with　high　desulfurization　efficiency　and　a　rapid　regeneration　ability,　thus　achieving　excellent　desulfurization　performance　in　a　slurry　reactor.　FeOOH-3　gives　a　H2S　breakthrough　capacity　of　55.1%,　which　is　far　higher　than　that　of　commercial　FeOOH.　More　importantly,　after　the　fourth　to　sixth　regenerations,　the　FeOOH-3@Fe-EDTA　displays　steady　performance　in　the　initial　20　min,　constantly　displaying　an　outlet　H2S　concentration　close　to　0　ppm.　©　2021　American　Chemical　Society