Strontium(II)-added CaAl2O4 composites prepared by sol-gel technique were investigated for the sensitive properties of volatile organic compounds (VOCs) like benzene, toluene, cyclohexane, hexane, and acetone. X-ray diffraction, scanning electron microscopy (SEM), FT-IR spectroscopy, and nitrogen adsorption/desorption isotherm at 77 K were employed, respectively, to identify the structural phases, surface morphology, vibrational stretching frequencies, and Brunauer-Emmett-Teller (BET) surface area of the composites. The composites were prepared with the molar ratios of Ca/Sr as (1.0:0.0-0.0:1.0), keeping the aluminum molar ratio as constant, and were labeled as CaSA1, CaSA2, CaSA3, CaSA4, CaSA5, and CaSA6, respectively. The samples, sintered at 900 °C for 5 h, were subjected to dc resistance measurements in the temperature range from 30 to 200 °C to study the VOC vapor-sensing characteristics. The results revealed that the sensitivity factor increased with an increase in temperature up to 150 °C and thereafter decreased. The sensitivity was found to increase with an increase in VOC concentration from 100 to 5000 ppm at 150 °C. Among the materials investigated, CaSA5 showed the best sensitivity at an operating temperature of 150 °C. © 2007 American Chemical Society.