The removal of highly radioactive and long-lived 137 Cs + and 90 Sr 2+ from solution is of significance for radionuclide remediation. Herein we prepared a two-dimensionally microporous thiostannate, namely (Me 2 NH 2 ) 4/3 (Me 3 NH) 2/3 Sn 3 S 7 $1.25H 2 O (FJSM-SnS), and systematically investigated its Cs + and Sr 2+ ionexchange performance in different conditions. The structural stabilities and variation, ion-exchange kinetic and isothermal behavior, pH-dependent distribution coefficients (K d ), ion-exchange in simulated groundwater and ion-exchange applied to chromatography have been investigated. The results indicated that the maximum Cs + and Sr 2+ ion-exchange capacities of FJSM-SnS were 408.91 mg g À1 and 65.19 mg g À1 , respectively. In particular, FJSM-SnS showed quick ion-exchange ability and wide pH resistance (0.7-12.7) which make it outstanding among the ion-exchangers. An ion-exchange chromatographic column was firstly studied for chalcogenido ion-exchange materials, that is, a column filled with 3.0 g FJSM-SnS could remove 96-99% of Cs + ion and near 100% of Sr 2+ ion at low ionic concentrations in 900 bed volumes solutions. Furthermore, the title material could be synthesized on a large scale by a facile, one-pot and economical solvothermal method. The relatively low cost but remarkable ion-exchange performance makes it promising for radionuclide remediation. † Electronic supplementary information (ESI) available: Crystallographic data for FJSM-SnS and FJSM-SnS-Cs in CIF format, TG-MS spectra, mass spectra of solution and solvent, PXRD, EDS, the kinetics studies at room temperature, IR and table of data in the simulated groundwater, competitive ion-exchange experiments and the ion-exchange chromatographic column experiment. CCDC 1025383 and 1025384. For ESI and crystallographic data in CIF or other electronic format see