This work presents a simple process for the development of flexible acetone gas sensors based on zinc oxide/graphene/poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate). The gas sensors were prepared by inkjet printing, which was followed by a metal sparking process involving different sparking times. The successful decoration of ZnO nanoparticles (average size ~19.0 nm) on the surface of the graphene-PEDOT:PSS hybrid ink was determined by characterizations, including Raman spectroscopy, Fourier transform infrared spectroscopy, field-emission transmission electron microscopy, X-ray photoelectron spectroscopy, and X-ray diffractometry. The ZnO nanoparticle-decorated graphene-PEDOT:PSS with a sparking time of 2 min exhibited the highest response of 71.9% at 10 ppm of acetone, above those of samples treated with other sparking times and the undecorated control. In addition, the optimal sensor revealed high selectivity for acetone over several other kinds of gases, such as ammonia, toluene, dimethylformamide, ethanol, methanol, and benzene, at room temperature. The gas sensor also revealed a low limit of detection (0.4 ppm), high sensitivity (6.18 ppm), and high stability (5-week long-term) to acetone. The response and recovery times of the sensor were found to be 4.6 min and 4.2 min, respectively. The acetone-sensing mechanism was attributed to the formation of p-n heterojunctions, which were responsible for the significantly enhanced sensitivity.