The possible advantages of employing neon‐dominated gas mixtures in e‐beam laser cavities are discussed, and cross sections for selective excitation of N2+, CO+, and CO2+in charge‐transfer collisions between Ne2+and N2, CO and CO2are reported. The magnitudes of these cross sections (measured using beam techniques) compare favorably with analogous measurements involving He2+reactant ions, suggesting that laser action in neon‐dominated mixtures might be achieved. The addition of helium to the ion source was observed to increase the Ne2+beam current; however, the accompanying increased photon yield was greater than the percentage increase in the beam current, indicating that vibrationally relaxed Ne2+is preferred. It is suggested that ’’seeding’’ a neon‐filled e‐beam laser cavity with helium could increase the over‐all efficiency of such a device.