Smooth voids are achieved in an anisotropic Fe:LiNbO3 crystal with a high refractive index by use of a femtosecond laser-driven microexplosion method. Due to the anisotropy of the crystal, the maximum fabrication depth and the fabrication power threshold are different in different crystal directions, indicating that the direction perpendicular to the crystal axis is more suitable for thick three-dimensional structure fabrication. The dependence of the threshold power on the illumination wavelength shows that the microexplosion mechanism is caused by a two-photon absorption process. As a result, a near threshold fabrication method can be used to generate quasispherical voids.

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