This study considered the removal of strontium (Sr2+) from contaminated water using a filtration membrane that exhibits good mechanical strength, high adsorption capacity, and the ability to be regenerated and reused. Polyvinyl alcohol hydrogel membranes were prepared by crosslinking with sulfosuccinic acid in different ratios (2.5, 5, 10 and 20 mol% relative to the PVA monomer), named as PSA2.5, PSA5, PSA10 and PSA20. All PSA membranes showed good Sr2+ adsorption over a wide pH range (pH 2–12), and maintained rapid removal kinetics (> 95% Sr2+ recovered from 5 ppm Sr2+ within 4 h). Furthermore, the Sr2+ adsorption capacities of PSA2.5, PSA5, PSA10 and PSA20 were 27.6, 45.8, 56.3, and 55.3 mg/g, respectively, based on the Langmuir adsorption isotherm. From the four PSA membranes, PSA5 was selected for further filtration studies due to its favorable mechanical and adsorption properties. When filtering 5 ppm Sr2+ and 250 ppm Ca2+, corresponding to the Ca2+ concentration in the wastewater at the Fukushima nuclear plant, 87% Sr2+ was removed using the PSA5 membrane following multiple cycles of regeneration and reuse. Moreover, the tensile strength of the PSA5 membrane remained high (> 100 MPa) following five consecutive uses.