SrZrO3 ceramic with perovskite-type structure was synthesized by a conventional solid-state reaction method at 1500 °C for 3 h. The crystal structures were studied by x-ray diffraction (XRD), and lattice vibrational modes were obtained by Raman and Fourier transform far-infrared (FTIR) reflection spectroscopy. The dielectric properties of the samples were also measured. According to XRD data, the SrZrO3 ceramic displayed the orthorhombic structure Pbnm (62). The Raman spectrum with ten active vibrators can be fitted by the Lorentzian function, and the vibrators were assigned. Far-infrared spectrum with six infrared active modes was fitted by the four-parameter semiquantum models. Consequently, the modes were assigned as F1u (1) (102 cm−1), F2u (2) (120 cm−1), F1u (3) (140 cm−1), F3u (4)′ (228 cm−1), F3u (4)″ (287 cm−1), F1u (5) (326 cm−1), and F1u (6) (527 cm−1). The infrared mode F1u (1), that can be represented as the Sr–ZrO6 inverted translational vibration, has the highest contribution to the dielectric properties (permittivity and dielectric loss). The calculated data agree well with the measured values.