The Ba[(Ni0.7Zn0.3)(1/3)Nb-2/3]O-3 solid solutions were sintered at 1450, 1500, and 1550 A degrees C for 3 h, respectively, by conventional solid-state sintering method, so as to clarify the effect of the sintering temperatures on vibrational modes, crystal structures, and dielectric properties. Ceramics were characterized by X-ray diffraction (XRD), Raman spectroscopy and Fourier transform far-infrared reflection (FTIR) spectroscopy. Space group and crystal symmetry of Pm (3) over barm were determined by XRD. Lattice vibrational spectra, obtained by Raman and FTIR spectroscopy, show the correlation among polar phonon modes, crystal structures, and dielectric properties of Ba[(Ni0.7Zn0.3)(1/3)Nb-2/3]O-3 ceramics as a function of the sintering temperatures. The results demonstrate that the dielectric constant epsilon(r) reaches a maximum value of 35.713 at 1500 A degrees C and is related to Raman shifts of the A(1g)(O) modes and the FWHM values of the E-g(O) modes, the temperature coefficient of the capacitance tau(c), which gradually increases from -6 x 10(-6)/A degrees C to 0, is closely related to the Raman shifts of E-g(O) modes, and the dielectric loss values are closely connected with the full width at half-maximum of E-g(O) active modes and the Raman shifts of of the A(1g)(O) modes with the increasing temperatures. FTIR shows that the dielectric properties are closely related to the far-infrared phonon modes. Raman and FTIR active modes were indicated according to the group theory.