Multidimensional NMR spectroscopy has been developed for correlating anisotropic interactions of different spins in solids rotating at the magic angle. Anisotropic interactions, such as heteronuclear dipolar couplings and chemical-shift anisotropies, are recovered in the evolution periods by newly designed RF pulse sequences. Calculated spectra for this correlation experiment depended on the mutual orientation of tensorial interactions. Thus, this method can provide structural-information, e.g., dihedral angles, for spin pairs distinguished by isotropic chemical shift. Experimental and numerically simulated results are presented for L-alanine fully labeled with C-13 nuclei. (C) 1997 Academic Press.