Structural, optical and microwave dielectric properties of Ca(1-x)sr(x)MoO(4) (x= 0.0, 0.2, 0.4, 0.6, 0.8 and 1.0) compositions were studied with help of Rietveld refinement and Raman spectroscopy measurements. All these compositions were prepared by solid state reaction method and observed to possess tetragonal scheelite structure with I4(1)/a space group. Microwave dielectric properties such as dielectric constant (epsilon(r)), quality factor (Qxf) and temperature coefficient of resonant frequency (tau(f)) were measured using Hakki-Coleman method, reflection technique and invar cavity attached to hot plate respectively. epsilon(r) (Q x f) and tau(f) are correlated with molar volume (V-m), Mo-O bond strength and Raman shift of A(1g) mode respectively. All these compounds show good microwave dielectric properties (epsilon(r) = 6.7-9.6, Q x f = 35,000-52,000 GHz and tau(f)= -28 to -17 ppm/degrees C). Band gap of these compositions was observed in the range 3.3-3.5 eV and variation in band gap was fitted with Bowing equation. (C) 2014 Elsevier Ltd. All rights reserved.