With the increasing demand for ammonia applications, there is a significant focus on improving NH3 detection performance at room temperature. In this study, we introduce a groundbreaking NH3 gas sensor based on Cu(I)-based coordination polymers, featuring semiconducting, single stranded 1D-helical nanowires constructed from Cu-Cl and N-methylthiourea (MTCP). The MTCP demonstrates an exceptional response to NH3 gas (>900% at 100 ppm) and superior selectivity at room temperature compared to current materials. The interaction mechanism between NH3 and the MTCP sensor is elucidated through a combination of empirical results and computational calculations, leveraging a crystal-determined structure. This reveals the formation of NH3-Cu and NH3-H3C complexes, indicative of a thermodynamically favorable reaction. Additionally, Ag-doped MTCP exhibits higher selectivity and a response over two times greater than the original MTCP, establishing it as a prominent NH3 detection system at room temperature.