In this study, MnO2/zeolite composites (MnO2@Z4As) were synthesized via a one-pot self-assembly reaction using low-cost kaolinite minerals as the starting material. The successful embedding of MnO2 nanoparticles within the zeolite matrix was confirmed through structural characterization. The highest capacity for Sr2+ adsorption was observed for MnO2@Z4A-9 at 177.49 mg/g, representing a 39.96% increase compared to zeolite 4A (Z4A) alone. The process displayed characteristics consistent with the Langmuir model and pseudo-second-order kinetic behavior, indicating that the adsorption was monolayer chemisorption. However, competing ions, such as Ca2+ and Na+, significantly hindered Sr2+ adsorption. In seawater, MnO2@Z4A-9 removed 98.4% of Sr2+ at a 10 g/L dosage. The dual adsorption mechanism of Sr2+ adsorption on MnO2@Z4As has been elucidated, comprising ion exchange with Na+ in the zeolite and the hydroxyl complexation with MnO2. This study offers a cost-effective strategy for Sr2+ removal from seawater.