Pure zinc oxide nanoparticles, as well as those doped with 3% calcium, aluminum, and gallium, were synthesized using a sol-gel method and then deposited onto an alumina substrate for sensing tests. The resulting nanoparticles were characterized using a variety of techniques, including X-ray diffraction (XRD), scanning electron microscopy (SEM) equipped with energy dispersive X-ray analysis (EDX), transmission electron microscopy (TEM), UV-VIS-NIR absorption spectroscopy, and photoluminescence (PL) measurements, to examine their structural, morphological, and optical properties. The prepared nanoparticles were found to have the hexagonal wurtzite structure of ZnO with a P63mC space group. The UV-Vis-IR spectra showed that the samples are highly absorbent in the UV range, while the PL spectra confirmed the presence of many defects in the ZnO structure, such as oxygen vacancies and zinc interstitials. The doped samples exhibited more defects than the pure sample. SEM images of the deposited film surface showed agglomerates with a spherical shape and confirmed the nanometer scale size of our prepared samples, as corroborated by the TEM images. The EDX spectra indicated the high purity of the ZnO deposited films, with a high presence of Zn and O and the presence of the doped elements (Ca, Al, and Ga) in each doped sample. Sensing tests were performed on ZnO, Ca3%-doped ZnO (C3ZO), Al3%-doped ZnO (A3ZO), and Ga3%-doped ZnO (G3ZO) sensors in the presence of volatile organic compounds (VOCs) gases such as ethanol, formaldehyde, methanol, and acetone at low concentrations. The sensors exhibited high responses to low ppm level concentrations of the VOCs gases. At a low operational temperature of 250 °C, the C3ZO sensor had the highest response to 5 ppm of ethanol, methanol, and formaldehyde gases compared to the pure and other doped sensors. Additionally, the A3ZO sensor exhibited the highest response to acetone gas. In conclusion, our findings suggest that the doping of zinc oxide can enhance the low concentration detection of VOCs gases, with the C3ZO and A3ZO sensors showing the highest response to specific gases.