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 degrees C for 5 h, were subjected to dc resistance measurements in the temperature range from 30 to 200 degrees C to study the VOC vapor-sensing characteristics. The results revealed that the sensitivity factor increased with an increase in temperature up to 150 degrees C and thereafter decreased. The sensitivity was found to increase with an increase in VOC concentration from 100 to 5000 ppm at 150 degrees C. Among the materials investigated, CaSA5 showed the best sensitivity at an operating temperature of 150 degrees C.