In view of the characteristics and risks of ammonia, its removal is important for industrial production and environmental safety. In this study, viscose-based activated carbon fiber (ACF) was used as a substrate and chemically modified by nitric acid impregnation to enhance the adsorption capacity of the adsorbent for ammonia. A series of modified ACF-based adsorbents were prepared and characterized using BET, FTIR, XPS, and Boehm titration. Isotherm tests (293.15 K, 303.15 K, 313.15 K) and dynamic adsorption experiments were performed. The characterization results showed that impregnation with low concentrations of nitric acid not only increased the surface acidic functional group content but also increased the specific surface area, while impregnation with high concentrations of nitric acid could be able to decrease the specific surface area. ACF-N-6 significantly increased the surface functional group content without destroying the physical structure of the activated carbon fibers. The experimental results showed that the highest adsorption of ammonia by ACFs was 14.08 mmol-L−1 (ACF-N-6) at 293 K, and the adsorption capacity was increased by 165% compared with that of ACF-raw; by fitting the adsorption isotherm and calculating the equivalent heat of adsorption and thermodynamic parameters using the Langmuir–Freundlich model, the adsorption process could be found to exist simultaneously. Regarding physical adsorption and chemical adsorption, the results of the correlation analysis showed that the ammonia adsorption performance was strongly correlated with the carboxyl group content and positively correlated with the relative humidity (RH) of the inlet gas. This study contributes to the development of an efficient ammonia adsorption system with important applications in industrial production and environmental safety.