This study reports the use of tin oxide (SnO2) octahedral nanoparticles with exposed high-energy facets as sensing material in inkjet-printed carbon monoxide (CO) gas sensors. The nanoparticles were synthesized via a hydrothermal method aimed at encouraging high-indexed (221) crystal planes to be exposed as facets, since their high surface energy may encourage interactions with gases. Studies by X-ray diffraction (XRD) confirmed the identity of the SnO2, while transmission electron microscopy (TEM) revealed formations of octahedral-shaped SnO2 nanoparticles, with features confirming the exposure of high-energy (221) crystal facets. The nanoparticles’ reductive behavior in a CO environment was studied using temperature-programmed reduction (TPR). A stable ink based on the SnO2 nanoparticles was successfully prepared and utilized to fabricate, via inkjet printing, homogenous films onto electrically conductive graphene-based interdigitated electrodes. Optimizing the inkjet printing parameters enhanced the CO gas sensing performance of the fabricated sensors. For example, at 200 ppm, the sensor with 10 printed layers recorded a sensitivity of about 20%, as compared to a sensitivity of not more than 14% recorded in each of the sensors with 5, 15, and 20 printed layers. As a result of having homogenous films, the inkjet-printed sensors also exhibited almost double the sensitivity of similar sensors prepared by drop-casting method.