Low power consumption, fast response and quick recovery times are important parameters for gas sensors performance. Herein, we report the experimental and theoretical studies of ZnO and Cr doped ZnO nanostructures used in low temperature (50 °C) sensors for the detection of CO. The synthesized films were characterized by XRD, UV-Vis, FE-SEM and EDX. The XRD patterns for the ZnO and 0.5 wt% Cr/ZnO films confirm the formation of a single-phase hexagonal wurtzite structure. The reduction of the ZnO optical band gap from 3.12 eV to 2.80 eV upon 0.5 wt% Cr doping is well correlated with the simulation data. The FE-SEM images of the films show spherical morphology with the estimated particle sizes of about ~40 nm and ~ 25 nm were recorded for the ZnO and 0.5 wt% Cr/ZnO films, respectively. Enhanced gas sensing performance is achieved with Cr doping and the sensitivity of ZnO increases from 9.65% to 65.45%, and simultaneously decreasing the response and recovery times from 334.5 s to 172.3 s and from 219 s to 37.2 s, respectively. These improvements in gas sensing performance are due to the reduction in particle size and optical band gap, and an increase in specific surface area.