The results of optical study and quantum-chemical simulation of a conjugated organic system, 2-cyclooctylamino-5-nitropyridine (COANP)-fullerene, performed to determine its potential for application as a limiter of visible and near-IR laser radiation and as a material for diffraction elements in systems for reversible recording of optical information, are presented. Complexation between a COANP molecule and fullerene is considered as one of the main mechanisms responsible for the corresponding properties of this system. For the first time, nonlinear optical characteristics of COANP-C60 and COANP-C70 systems are comparatively studied and the intermolecular interaction between a COANP molecule and fullerene is analyzed on the quantum-chemical level. © 2004 MAIK "Nauka/Interperiodica".