A Nd:Cr:YVO4 crystal was grown by the Czochralski method for the first time to our knowledge. Its structure and cell parameter have been studied by X-ray powder diffraction (XRPD) analysis. Polarized absorption spectra were measured at room temperature, which showed that the absorption bands display polarization character and an absorption band of Cr5+ ions at 1110 nm enables the crystal to be a self-Q-switched laser material. We also found that the absorption of Cr5+ ions became much larger and its self-Q-switched laser performance became much better when the Nd:Cr:YVO4 crystal was annealed because the annealing induces more Cr ions to become those with + 5 valence. In the self-Q-switched laser, the maximum output power, shortest pulse width, and largest pulse energy were obtained to be 120 mW, 85.8 ns, and 0.79 μJ, respectively.