The efficient, selective, and economical sorbents for the removal of Sr radionuclides are largely needed for the decontamination of effluents with high salinity. In this study, the removal of Sr was investigated using the zeolite produced from the Bayer process liquids. Based on the XRD, SEM/EDS analysis, the product was pure and highly crystalline zeolite 4A (Z4A). Removal of Sr was fast (5 min for 100% removal at 8.80 mg/L), with high maximum sorption capacity (252.5 mg/L), and independent on the initial pH in the range 3.5–9.0. Specific sorption of Sr by protonated groups on the Z4A surface was operating in addition to ion-exchange with Na ions. The selectivity of Z4A decreased in the order Sr > Ca > K > Mg > Na. 84% of Sr was separated from seawater within 5 min, at the Z4A dose of 5 g/L, while efficiency increased to 99% using the dose of 20 g/L. Desorption of radioisotope 89Sr from seawater/Z4A solid residue was very low in deionized water (0.1–0.2%) and groundwater (0.7%) during 60 days of leaching. Z4A is a cost-effective, selective, and high-capacity medium for Sr removal, which provides high stability of retained radionuclides.