Unconventional　ion　exchangers　can　achieve　efficient　removal　of　[UO2]2+,　Cs+,　and　Sr2+　ions　from　complex　aqueous　solutions　and　are　of　great　interest　for　environmental　remediation.　We　report　two　new　gallium　thioantimonates,　[Me2NH2]2[Ga2Sb2S7]·H2O　(FJSM-GAS-1)　and　[Et2NH2]2[Ga2Sb2S7]·H2O　(FJSM-GAS-2),　which　present　excellent　ion　exchange　properties　for　[UO2]2+,　Cs+,　and　Sr2+　ions.　They　exhibit　high　ion　exchange　capacities　for　[UO2]2+,　Cs+,　and　Sr2+　ions　(qmU　=　196　mg/g,　qmCs　=　164　mg/g,　and　qmSr　=　80　mg/g　for　FJSM-GAS-1,　qmU　=　144　mg/g　for　FJSM-GAS-2)　and　short　equilibrium　times　for　[UO2]2+　ion　exchange　(5　min　for　FJSM-GAS-1　and　15　min　for　FJSM-GAS-2,　respectively).　Both　compounds　display　active　ion　exchange　with　[UO2]2+　in　the　pH　range　of　2.9-10.5.　Moreover,　the　sulfide　compounds　could　maintain　high　distribution　coefficients　KdU　even　in　the　presence　of　excess　Na+,　Ca2+,　and　HCO3-.　The　distribution　coefficient　KdU　of　6.06　×　106　mL/g　exhibited　by　FJSM-GAS-1　is　the　highest　among　the　reported　U　adsorbents.　The　[UO2]2+-laden　products　can　be　recycled　by　conveniently　eluting　the　uranium　with　a　low-cost　method.　These　advantages　combined　with　facile　synthesis,　as　well　as　β　and　Î　radiation　resistance,　make　FJSM-GAS-1　and　FJSM-GAS-2　promising　for　selective　separations　in　nuclear　waste　remediation.　©　Copyright　2018　American　Chemical　Society.