Single phase materials of PbZr1-xTixO3 (x = 1.00, 0.65 and 0.35) were prepared by following the solid state route. All the materials were prepared in nanocrystalline form as well as microcrystalline form. Evolution of crystallization was studied by characterizing the samples annealed at different temperatures. XRD patterns were analyzed with the help of Fullprof program by employing Rietveld refinement technique. The patterns for x = 1.00 and 0.65 could be refined using P4mm space group in tetragonal symmetry. However, the samples for x = 0.35 could be refined using R3c space group in rhombohedral symmetry. It has been found that crystallite size increases with the annealing temperature for all the samples. The scanning electron microscope (SEM) and energy dispersive X-ray spectroscope (EDS) analysis reveals that the materials are uniform and their composition is as per the chemical formulae. All the samples exhibit ferroelectric to paraelectric transition. (C) 2010 The Society of Powder Technology Japan. Published by Elsevier B.V. and The Society of Powder Technology Japan. All rights reserved.