We report an experimental and theoretical investigation of electron-impact single ionization of the HOMO 1t 2 and the NHOMO 2a 1 states of CH 4 at an incident electron energy of 250 eV. Triple differential cross sections measured in two different laboratories were compared with results calculated within the molecular 3-body distorted wave (M3DW) and generalized Sturmian function (GSF) theoretical models. For ionization of the 1t 2 state, the binary peak was observed to have a single maximum near the momentum transfer direction that evolved into a double peak for increasing projectile scattering angles, as has been seen for ionization of atomic p-states. A detailed investigation of this evolution was performed. As expected because of its s-type character, for ionization of the 2a 1 state only a single binary peak was observed. Overall, good agreement was found between experiment and theory.