A complex study of the microstructure of titanium and zirconium pseudo-single crystals subjected to severe plastic deformation in Bridgman anvils under a pressure of 8 GPa at a temperature of 80 K has been carried out. Raman spectra of the samples deformed to different degrees show a two-phase α + ω state, which indicates the realization of the pressure-induced transition during deformation process with the retention of the ω-phase in the structure of both metals after the load removal. The quantitative ratio of α- and ω- phases in the structure of deformed metals and its change with increasing degree of deformation has been analyzed. Correlation of Raman spectroscopy results with experimental data of X-ray diffraction analysis, electron microscopic analysis, as well as literature data of calorimetry and calculated thermodynamic data by DFT method on kinetics of the reverse ω → α transformation demonstrates the efficiency of Raman spectroscopy method for estimation of the phase composition of pure metals, which experienced phase transition under loading.