We report on the crystal growth, optical spectroscopy, and 2-µm laser operation of co-doped Tm3+/Ho3+:SrMoO4 scheelite crystals. High optical quality crystals co-doped with Tm3+ (7.9×1019cm−3) and Ho3+ (8.0×1019cm−3) were grown from the melt in air by the Czochralski method. We characterized the spectroscopy of Tm3+ and Ho3+ ions in SrMoO4 in terms of polarized optical absorption, photoluminescence, and lifetime. Pulsed diode-pumped laser operation at room temperature at a wavelength of 2.06μm was achieved with a maximum output power of 1.62mW and a slope efficiency of 3%. The results showed that Tm3+/Ho3+:SrMoO4 crystals can be a promising material for developing a diode pumped mid-IR laser with Raman self-conversion of radiation in the active medium.