A Nd3+-doped Ca9Y(VO4)7 crystal with high optical quality and dimension of φ30 mm×35 mm has been grown by the Czochralski method. The effective segregation coefficient of Nd3+ ion is measured as 0.75. The parameter of second-order nonlinear optical coefficient of the powder is 1.5 times as large as that of KDP crystal. Its Vickers hardness is 362. The spectral properties of Nd3+Ca9Y(VO4)7 crystal have been investigated that the absorption cross section is 1.50×10-19 cm2 with full width half maximum (FWHM) of 13 nm at 809 nm, which fits to be pumped by GaAlAs laser diode. The emission cross section is 1.35×10-20 cm2 and the fluorescence lifetime is 103 μs at the highest emission peak of 1069 nm. The results show that the Nd3+Ca9Y(VO4)7 crystal is a new self-frequency-doubling crystal.