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The complexation of a cylindrical polyelectrolyte–brush-surfactant complex (PMMPSS–C12) and an oppositely charged generation-5 PAMAM dendrimer (G5-PAMAM) in methanol (MeOH) leads to kinetically controlled formation of interpolyelectrolyte complexes. In contrast, the complexation of the same starting materials in solvents with higher dielectric constant such as dimethylformamide (DMF) or N-methylformamide (NMF) results in the formation of topologically controlled complexes of cylindrical morphology. The composition of the complexes is analyzed by static and dynamic light scattering (SLS, DLS) in solution and atomic force microscopy (AFM) after spin-casting the complexes onto mica. The analyzed complexes seem to consist of one PMMPSS–C12 molecule and, with increasing G5-PAMAM content, of an increasing number of G5-PAMAM dendrimers.