Nd1-xSmx(Mg0.5Ti0.5)O 3 (x = 0.0-1.0) samples were prepared by solid-state reaction method. Rietveld refinement of X-ray diffraction data was done using P21/n space group with monoclinic symmetry, which supports 1:1 B-site cation ordering. Long range ordering (LRO) parameter decreased up to x = 0.5 and then found to increase with further increase in Sm concentration. The A1g-like mode in Raman spectra was observed to possess Briet-Wigner-Fano line shape. The variation in obtained line width of the A1g-like mode supported LRO. Microwave dielectric characteristics such as dielectric constant (εr), quality factor (Q) and temperature coefficient of resonant frequency (τf) were measured in the range of 7-9 GHz. εr decreased from 26.5 to 24.9 and τf become less negative from -58 ppm/°C to -36 ppm/°C with increase in Sm concentration. Q × f decreased from 47,500 GHz (for x = 0) to 39,800 GHz (for x = 0.5) and then increased to 44,600 GHz (for x = 1). © 2012 Elsevier Ltd.