The two- and three-photon resonant spectra of CH3Cl have been recorded in the region of the lower Rydberg states. Assignments are made for numerous electronic and vibrational bands related to the first two members of the s, p, and d Rydberg series in CH3Cl, extending or revising the assignments of previous workers. Comparisons of two- and three-photon spectra and polarization effects show strong contrast and reveal the varying degrees of atomic behavior in the six electronic states studied. The orbital angular momentum quantum number of the Rydberg state is shown to have a greater influence on the degree of penetration and consequent deviation from hydrogen-like orbital character than the magnitude of the principal quantum number.