The complete set of second-order nonlinear optical (NLO) coefficients of Cs2TeMo3O12 single crystals were obtained using the Maker Fringe techniques. The NLO coefficients d32 and d33 were measured to be on the order of 6.8 and 6.5 pm/V, respectively. Irradiated by 1064 nm laser, the crystal is phase-matchable, and its effective nonlinear coefficient is 4.6 pm/V for type I phase matching at θ = 42.7°. The relationship between the second-order nonlinear properties and the crystal structure is also discussed. Considering its wide transmission range, phase matching, and large effective NLO coefficient, Cs2TeMo3O12 is a good candidate for IR NLO application.