Pure and urea-modified zinc oxide thin films are prepared using the spray pyrolysis technique on microscopic glass substrates. We have added different urea concentrations as a modifier to the zinc acetate precursor for obtaining urea-modified ZnO thin films and investigated the effect of the urea concentration on the structural, morphological, optical, and gas-sensing properties. The gas-sensing characterization of pure and urea-modified ZnO thin films is tested in the static liquid distribution technique with 25 ppm of ammonia gas at an operating temperature of 27 °C. The prepared film with a concentration of 2 wt % of urea has shown the best sensing properties toward ammonia vapors due to more active sites for the reaction between chemiabsorbed oxygen and the target vapors.