In this study, sol-gel synthesis conditions for the formation of La2-xSrxNiO4 (x = 0, 0.2, 0.4, 0.6, and 0.8) compounds were investigated. Effects of Sr substitution on A-site on the properties of the compounds were studied using Fourier transform IR spectroscopy, X-ray diffractometry, scanning electron microscopy, and electrical and thermal analyses. A simple sol-gel preparation process was successfully developed at room temperature using water as the solvent in the presence of ethanolamine as the directing agent. The sol-gel synthesis method was effective in yielding higher purity and more homogenous samples than those synthesized via the solid-state reaction method. The addition of Sr helped stabilize the Ruddlesden-Popper structure, and a highly agglomerated morphology of the sintered samples with Sr substitution was observed, resulting in lower density. Sr helped increase conductivity, whereas its effect on thermal expansion was not as pronounced. La1.2Sr0.8NiO4 synthesized via the sol-gel process provided a conductivity of 160 S/cm at 500 degrees C with a coefficient of thermal expansion value of 13 X 10(-6)degrees C-1 between 400 and 700 degrees C. (c) 2010 The Electrochemical Society. [DOI: 10.1149/1.3489262] All rights reserved.