Polarized laser photolysis of ICN is combined with saturated optical pumping to prepare state-selected CN A2? (?' = 4, J = 0.5, F2, f) with a well-defined anisotropic superthermal speed distribution. The collisional evolution of the prepared state is observed by Doppler-resolved Frequency Modulated (FM) spectroscopy via stimulated emission on the CN A2?-X2S+ (4,2) band. The phenomenological rate constants for removal of the prepared state in collisions with He, Ar, N2 and O2 are reported. The observed collision cross-sections are consistent with attractive forces contributing significantly for all the colliders with the exception of He. The collisional evolution of the prepared velocity distribution demonstrates that no significant back-transfer into the prepared level occurs, and that any elastic scattering is strongly in the forward hemisphere. © the Owner Societies 2007.