A mechanism for sustaining population inversions in contact charge‐transfer complexes in which the ground electronic state is not bound is described. The mechanism relies on picosecond radiationless depletion of the lower laser state. This generates an inversion even when the ground‐state potential curve, as plotted against the donor‐acceptor distance, is not repulsive vertically below the excited state minimum. Contact charge‐transfer lasers would offer high gain, high‐energy density, and tunable sources of coherent radiation in the uv and visible. A method for pumping such a laser is examined and applied to the pyrrole‐oxygen complex. A rate equation analysis is done and estimates for gain and energy density are presented.