Raman spectral features associated with the reorganization of solvent molecules around a solute are obtained using multivariate curve resolution. Spectra collected from solutions of variable concentration are resolved into unperturbed and perturbed components assuming only that the spectra and concentrations of each component are non-negative (with no peak-fitting or constraints on the shapes of either the perturbed or unperturbed spectral features). The capabilities of the method are demonstrated using solutions of acetonitrile, acetone, and pyridine in water as well as acetonitrile and cyclohexane in 1,2-dichloroethane (DCE). The results reveal vibrational spectra of solvation-shell molecules that are perturbed by each solute. The perturbed solvent-shell water molecules are found to have different OH stretch bands (of higher frequency and narrower width than bulk water), and the gauche-trans equilibrium of solvent-shell DCE molecules are perturbed in opposite directions by the polar and nonpolar solutes.