We investigated the effects of Co doping on the NO gas sensing characteristics of ZnO-carbon nanotube (ZnO-CNT) layered composites fabricated by coaxial coating of single-walled CNTs with ZnO using pulsed laser deposition. Structural examinations clearly confirmed a distinct nanostructure of the CNTs coated with ZnO nanoparticles of an average diameter as small as 10 nm and showed little influence of doping 1 at.% Co into ZnO on the morphology of the ZnO-CNT composites. It was found from the gas sensing measurements that 1 at.% Co doping into ZnO gave rise to a significant improvement in the response of the ZnO-CNT composite sensor to NO gas exposure. In particular, the Co-doped ZnO-CNT composite sensor shows a highly sensitive and fast response to NO gas at relatively low temperatures and even at low NO concentrations. The observed significant improvement of the NO gas sensing properties is attributed to an increase in the specific surface area and the role as a catalyst of the doped Co elements. These results suggest that Co-doped ZnOCNT composites are suitable for use as practical high-performance NO gas sensors.