For the nuclear industry, uranium is not only an important strategic resource but also a serious global contaminant with radiotoxicity and high chemotoxicity. It is very important to efficiently capture uranium from complex aqueous solutions for further treatment and disposal of nuclear wastes. Herein, we first demonstrate the suitability of a three-dimensional (3D) water-stable K+-exchanged zeolitic sulfide, namely K@GaSnS-1, for the remediation of radioactive and toxic uranium by ion exchange. In comparison to the pristine compound GaSnS-1, the K+-activated porous sulfide K@GaSnS-1 exhibits faster [UO2](2+) ion uptake kinetics, following the pseudo-second-order adsorption model. Further studies indicate that K@GaSnS-1 shows high exchange capacity (q(m)(U)= 147.6 mg/g) and wide pH resistance (pH 2.75-10.87). In particular, it can efficiently capture [UO2](2+) ion even when excessive amounts of Na+, K+, Mg+, and Ca+ ions are present. The highest distribution coefficient value K-d, signifying the affinity and selectivity for [UO2](2+) ion, reaches as high as 1.24 x 10(4) mL/g. More importantly, the uranium in corresponding exchanged samples can be facilely and effectively eluted by a low-cost and eco-friendly method. These merits of K@GaSnS-1 make it promising for the effective and selective removal of uranium from complex contaminated water.