The second order nonlinear optical properties of BaTeMo2O9 were studied by means of Maker fringe technology and the phase matching method. The value and relative sign of the second order nonlinear optical coefficients were obtained, with the largest being d31 = 9.88 pm/V. At 1064 nm, the crystal can support noncritical phase-matching, and the effective nonlinear coefficient is 10.3 pm/V for phase matching II at (90°, 62.8°) in the x0y plane. The relation between the second order nonlinear properties and the crystal structure is also discussed. All the results show that BaTeMo2O9 is a good candidate for nonlinear optical applications.