AbstractWith the increasing awareness of the hazards associated with ammonia (NH3) contamination and the potential application of NH3 detection in physical health monitoring, the exploration of high‐performance NH3 sensors has attracted significant attention in recent years. In this paper, we prepared copper iodide (CuI) nanomaterials combined with CuI‐isopropanolamine (C3H9NO) complexes by dissolving CuI in C3H9NO and subsequent annealing. The resulting product demonstrated exceptional sensing performance to 0.15 (mole fraction) NH3, exhibiting a maximum response of 7.5×105 with a response time of 5 s. The achieved detection limit was 10 ppm. Our findings provide a valuable reference for further research on NH3 sensors utilizing complexes formed by copper compounds and organic amines.