A method to measure the rotational diffusion coefficients of a liquid crystal based on the measurements of auto and cross-correlated relaxation is presented here. We report the measurements of cross-correlations between the relaxation processes originating from the chemical shift anisotropy (CSA) of C-13 and its dipolar coupling with the attached proton, for various carbons in a liquid crystal. The spectral densities are expressed as a function of motional parameters, using extended Lipari-Szabo model-free approach. These motional parameters were extracted from the measured self-relaxation, cross-relaxation and the cross-correlation rates. The potential of this method is demonstrated by the determination of the rotational diffusion coefficients of N-4-methoxybenzylidene-4-butylaniline (MBBA) at 297 K undergoing magic angle sample spinning. (C) 2003 Elsevier Science B.V. All rights reserved.