Broadband three-stage frequency conversion of multiline sub-microsecond CO laser radiation in a single sample of ZnGeP2 crystal was experimentally and numerically studied for the first time, to the best of our knowledge. As a result, the hybrid laser system emitted more than 200 narrow spectral lines within the 2.4–6.2 μm spectral range. The measured conversion efficiencies of the first, second, and third stages were about 4.8%, 0.4%, and 0.05%, respectively. Our numerical simulation demonstrated that the third stage of this frequency conversion can extend the laser system spectrum toward the shorter wavelength of 2.2 μm.