A particulate sol-gel (PSG) process has been developed for synthesizing LiNiO2 and LiNi0.75Co0.25O2 powders. The process is a modified derivative of the colloidal sol-gel technique and yields a precursor that transforms to the oxide by heat treatment at a maximum temperature of 800 degrees C in only 2 h. The synthesized oxides also display good electrochemical activity (135 mA h/g for LiNiO2 and 182 mA h/g for LiNi0.75Co0.25O2) for application in lithium-ion rechargeable batteries. Detailed structural characterization of the as-prepared xerogels have been conducted using Fourier transform infrared spectroscopy (FTIR), while studying their phase evolution behavior during heat treatment using X-ray diffraction (XRD). Results of these studies have been described in this work.