The new nonlinear optical crystal MnTeMoO6 has been grown by the top-seeded solution growth method with sufficient size (15 mm×10 mm×4 mm) and optical quality that allowed the characterization of its properties. Powder second harmonic generation measurements indicate that MnTeMoO6 displays a large SHG response of approximately 0.7×KTP. Additional SHG measurements indicate the material is type-I phase-matchable. The full-width at half-maximum of the X-ray rocking curve on the (110) face of the as-grown crystal is 0.131°. Thermal analysis demonstrates that the MnTeMoO6 crystal melts congruently at 735.6 °C. Optical measurements indicate that the MnTeMoO6 crystal has a broad transmission window range from 0.41 to 5.4 μm. The Vickers-hardness value of the MnTeMoO6 crystal is 326.8 HV, which is equivalent to Mohs' hardness of about 5.