A new rheometrical technique has been developed to determine the mechanical relaxation spectra of viscoelastic materials by measurement of shear wave group and phase velocities in a virtual gap rheometer. The technique’s sensitivity and accuracy in providing relaxation spectra directly from measurements arises from exploitation of marked changes in wave dispersion characteristics in the vicinity of stress relaxation mechanisms. The new technique is compared with two conventional, wave-based rheometrical techniques (based on pulse-propagation and resonance measurements), which are adversely affected by wave dispersion. The superior accuracy and sensitivity of the new technique over conventional rheometry is demonstrated with reference to the Maxwell model and published relaxation spectra. Experimental results obtained on a concentrated colloidal dispersion serve to demonstrate the measurement principles.