Ternary complexes C60-tetraphenylporphyrin-poly(vinylpyrrolidone) were synthesized and characterized. The synthesis of these complexes allows the amount of a water-soluble C60 to be increased by ≈5 times compared to complexation of C60 with poly(vinylpyrrolidone). Using the methods of 13°C NMR spectroscopy and small-angle neutron scattering, it was shown that complexation occurs in a C60-tetraphenylporphyrin binary system; the composition of a C60-tetraphenylporphyrin (1:1) complex was established from isothermal translation diffusion measurements. According to hydrodynamic and electrooptical studies of ternary C60-tetraphenylporphyrin-poly(vinylpyrrolidone) systems, the polymer coil involved in the complexes of interest exhibits a higher symmetry compared to the free poly(vinylpyrrolidone). It was found that an increase in the content of C60 in the ternary complex leads to the appearance of aggregates in its aqueous solutions.