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The non-stoichiometric Nd[Mg1/2(1+x)Sn1/2]O3 (NMS, − 0.04 ≤ x ≤ 0.04) were synthesized through a routine solid-state reaction process. The phase composition, phonon characteristics, and microwave dielectric properties were investigated by X-ray diffraction patterns, Scanning electron microscopy Raman and Fourier transform far-infrared reflection. The best crystallinity with uniformly distributed grains and clear grain boundaries at x = 0.01. The intrinsic properties were calculated by four-parameter semi-quantum model based on far-infrared reflectivity data, which agree well with those values obtained from the microscopic polarizabilities & damping coefficient angle. The correlations between intrinsic properties and lattice vibrational modes were discussed in particular. [ABSTRACT FROM AUTHOR]