As a new type of separation material, two-dimensional membrane has attracted wide attention due to its special transport mechanism. However, due to the hydration swelling of montmorillonite nanosheets, there are still challenges in preparing two-dimensional membrane with stable channel structure and fixed interlayer spacing. In order to overcome the problems caused by swelling, this study used polyvinyl alcohol and polyacrylic acid to stabilize the channel structure of two-dimensional membranes. Moreover, the crosslinking between Fe3+ and montmorillonite nanosheets was proposed to fix the interlayer spacing of two-dimensional membrane. It is found that various polymers had different effects on the mechanical property of two-dimensional membrane. The addition of polyvinyl alcohol and polyacrylic acid can significantly improve the tensile strength of the membrane. And the introduction of them reduces the hydrophilicity of the membrane surface, thus improving the stability of the membrane in water. In addition, the interlayer cations affect the stability of interlayer spacing of the membrane in water. After crosslinking the membrane with Fe3+, the interlayer spacing is fixed and can be maintained at about 0.94 nm in water for a long time. When a certain dosage of polyvinyl alcohol and PAA are added into the membrane and the crosslinking conditions are suitable, two-dimensional membrane has good selectivity to Li+ and Mg2+ in high Mg/Li ratio brine. Inspired by the natural ion exchange properties of montmorillonite, this study found a new method for inhibiting the hydration swelling of two-dimensional membrane and realizing precise control of interlayer spacing.