The study that is reported here is concerned with the development of an experimental route to the four independent components of the electric dipole polarizability of species of C s symmetry and, in particular, with the specification of the anisotropic polarizabilities of NH 3 , CH 3 NH 2 , (CH 3 ) 2 NH, and (CH 3 ) 3 N, for which a consistent set of data has not been available. It is shown that the four equations required to evaluate the four components of the optical-frequency (λ ) 632.8 nm) polarizabilities of CH 3 NH 2 and (CH 3 ) 2 NH can be drawn from measurements of (1) the temperature dependence of the electrooptical Kerr effect, (2) the Rayleigh depolarization ratio, and (3) the refractive index of the gas together with (4) a simple bond-additivity model of the polarizability. The model uses the polarizabilities of the C 3V species NH 3 and (CH 3 ) 3 N to estimate the off-diagonal polarizabilities of the C s species CH 3 NH 2 and (CH 3 ) 2 NH. To this end, improved equipment has been used to record the vapor-phase Kerr effects of NH 3 , CH 3 NH 2 , (CH 3 ) 2 NH, and (CH 3 ) 3 N over ranges of temperature and pressure. An analysis of the data yields precise values of the anisotropic polarizabilities and, as a bonus, less precise values of the Kerr hyperpolarizabilities of all four molecules and provides a clear demonstration of the utility of the method.