NiO nanocones decorated with ZnO nanothorns on NiO foil substrates are shown to be an ammonia sensor with excellent comprehensive performance, which could, in real-time, detect and monitor NH3 in the surrounding environment. Gas-sensing measurements indicate that assembling nanocones decorated with nanothorns on NiO foil substrate is an effective strategy for simultaneously promoting the stability, reproducibility, and sensitivity of the sensor, because the NiO foil substrate as a whole can quickly and stably transfer electrons between the gas molecules and the sensing materials and the large specific surface area of both nanocones and nanothorns provide good accessibility of the gas molecules to the sensing materials. Moreover, p-type NiO, with majority charge carriers of holes, has higher binding affinity for the electron-donating ammonia, resulting in a significant increase in selectivity toward NH3 over other organic gases. Compared with the NiO nanowires and pure NiO nanocones, the heterogeneous NiO nanocones/ZnO nanothorns exhibit less dependence on the temperature and humidity in response/recovery speed and sensitivity of sensing NH3. Our investigation indicates that two factors are responsible for reducing the dependence on the gas sensing characteristics under various environmental conditions. One is that the n-type ZnO nanothorns growing on the surface of nanocones, with majority charge carriers of electrons, speed up adsorption and desorption of gas molecules. The other is that the abundant cone-shaped and thornlike superstructures on the substrate are favorable for constructing a hydrophobic surface, which prevents the gas sensing material from being wetted.