A quantum-chemical analysis of the donor-acceptor properties of a C 60 + dimethylenemethylamine binary system is performed. It is shown that the term of the intermolecular interaction is two-well, because of which the optimization of the system structure at the initial distances between the molecules of 0.21 nm or smaller leads to the formation of N- methylfullerenepyrrolidine C60. At initial distances exceeding 0.25 nm, a weakly bound charge transfer complex with almost complete retention of the properties of the individual molecules is formed. The low-temperature emission and absorption vibronic spectra of N-methylfullerenepyrrolidine C60 in the crystalline toluene matrix are studied experimentally. It is found that the absorption spectra of the fulleroid and pure fullerene in the region corresponding to the excitation of the lowest electronic states are generally similar. The difference observed between the low-frequency spectra agrees completely with the quantum-chemical analysis performed. © Nauka/Interperiodica 2007.