The controllable interactions of a spherical polymer brush modeled by a poly(styrene-b-4-vinylpyridinium methyl iodide)-polyoxometalate composite micelle, SVP-6, with a polyoxometalate-based supramolecular star polymer, PSP-4, in solvents of variable quality allow us to tune their self-assembly behaviors from self-recognition to supramolecular recognition. In the former case, isolated, contractive spheres together with a few vesicles formed by PSP-4 coexist with multimicelle aggregates formed by SVP-6, whereas SVP-6 is hosted inside the vesicle of PSP-4 in the latter case. This work represents an important step toward the development and understanding of programmable self-assembly of brushlike polymers into complex materials.