Infrared lasers pumped by electronic‐vibrational (E‐V) energy transfer are reported. Gas mixtures containing electronically excited Br atoms (2P1/2) are prepared by flash photolyzing Br2 in the presence of a polyatomic molecule. The ensuing E‐V process is selective and pumps the polyatomic molecule into specific energy states. In addition to obtaining gain and/or stimulated emission at CO2 and N2O laser frequencies, we have obtained stimulated emission from HCN at 3.85, 7.25, and 8.48 μm, and from C2H2 in the region 7–8 μm. Extension of the principles involved to other polyatomic molecules is straightforward, and a number of applications are suggested by our results to date.