The values of longitudinal nuclear spin relaxation rates for the Hg-199 (spin-1/2) and N-14 (spin-l) nuclei and of the quadrupolar cross-correlation coefficient for. the N-14 nuclei are determined for a toluene solution of bis(hexamethyldisilylamido)mercury(II) in a broad temperature range. Estimates of the latter quantity were obtained from iterative line shape ffts of the Hg-199 resonance signals. Sensitivity of the Hg-199 resonances to the quadrupolar cross-correlations is because in the temperature range investigated the quadrupolar relaxation rates of the N-14 nuclei become comparable to the Hg-199-N-14 scalar coupling. The data obtained are shown to be consistent with the structure in which the Si2N-Hg-NSi2 skeleton maintains D-2d geometry on the time scale of the overall molecular reorientation. Under a well-justified assumption involving the extent of the possible anisotropy of the latter, the principal axes of the N-14 electric field gradient tensors, corresponding to the gradients of maximum absolute values, can be unambiguously located along the direction of the N-Hg-N chain. The value of the electric field gradient asymmetry parameter, calculated from the experimental data assuming perfectly isotropic reorientation, amounts to 0.62. The present study seems to provide the first evidence of the utility of quadrupolar cross-correlation effects for structural studies in isotropic liquids.