The cation-induced aggregation of sandwich crown-substituted complexes [Ln(R4Pc)(2)] (Ln = Lu (I) and Yb (II), R4Pc2- is the 4,5,4',5',4 '',5 '',4''',5'''-tetrakis(1,4,7,10,13-pentaoxatridecamethylene)phthalocyaninate ion) and Ln(2)(R4Pc)(3)(Ln = Lu (III) and Yb (IV) in a CDCl3-DMSO-d(6) solution has been studied by H-1 NMR. The data obtained are consistent with the conclusions concerning the composition of supramolecular aggregates drawn from spectrophotometric titration data. The molecules of double-decker complexes I and II form supramolecular oligomers, whereas triple-decker complexes III and IV form supramolecular dimers, which is presumably due to the stronger distortion of the planes of the outer decks of the triple-decker complexes as compared to their double-decker analogues.