The electronic structure of the endohedral fullerene 14N@C60 spatially ordered in the crystal state by its supramolecular assembly with a buckycatcher C60H28 was investigated by X-band electron paramagnetic resonance (EPR) spectroscopy. The zero-field splitting (ZFS) found in the complex is significantly enhanced in comparison to the earlier reported data for the analogous systems. The large ZFS, presumably induced by the molecular order in the supramolecular complex makes it an attractive material for the future quantum control and coherence studies.