Paramagnetic endohedral fullerenes hold promise for quantum information processing. In the case of endohedral nitrogen fullerenes such as N@C₆₀ and N@C₇₀, the nitrogen atom is almost completely isolated from the fullerene cage. This results in very long electron spin phase coherence times. The chemistry of endohedral nitrogen fullerenes has developed to a degree where it can be used to create functionalized systems with high aspect ratios that are prone to high alignment. In this talk, I will present our recent results for several N@C₆₀ and N@C₇₀ derivatives that we have aligned in liquid crystals. Within the liquid crystal matrix, we have achieved an order parameter factor O_zz of 0.61. This is a significant improvement on the best result that has been previously reported for endohedral fullerene derivatives. More importantly, this allows us to manipulate the intrinsic zero-field splitting (ZFS) of the spin resonance signal. By in-situ rotating frozen endohedral fullerenes inside the magnetic field of the ESR spectrometer, we deliberately changed the orientation distribution of the molecules and tuned the splitting energy of ZFS. We achieved remarkable agreement between experimental values and simulation data. This work can be expanded to control of dipolar coupling for a two-qubit gate. Hence it is quite pertinent to research on potential applications of endohedral fullerenes.