Adaptive bionic self-correcting behavior offers an attractive property for chemical systems. Here, based on the dynamic feature of imine formation, we propose a solvent-responsive strategy for smart switching between an amorphous ionic polyimine membrane and a crystalline organic molecule cage without the addition of other building blocks. To adapt to solvent environmental constraints, the aldehyde and amine components undergo self-correction to form a polymer network or a molecular cage. Studies have shown that the amorphous film can be switched in acetonitrile to generate a discrete cage with bright birefringence under polarized light. Conversely, the membrane from the cage crystal conversion can be regained in ethanol. Such a membrane-cage interconversion can be cycled continuously at least 5 times by switching the two solvents. This work builds a bridge between the polymer network and crystalline molecules and offers prospects for smart dynamic materials.