The invention provides a method for preparing solation-gelation hybridized nano self-assembly aggregation. A polymethylacrylic acid gamma-trimethoxy silane ester macromolecular chain transfer agent regulates and controls reversible addition-fragmentation chain transfer polymerization of styrene in a selective solvent, so that the solation-gelation self-assembly aggregation with different shapes is prepared in an in-situ self-assembly manner. The self-assembly aggregation can stabilize a micellar structure or introduce functional hybridized components through further solation-gelation.