Amines have received increasing attention in recent years because of their potential role in new particle formation in the atmosphere and their impact on aerosol chemistry. High concentrations of amines are expected to be limited to the vicinity of source regions due to their short lifetime, highlighting the necessity of having a better understanding of contributions of emissions from different source types. This study presents the first high-resolution model simulation of methylamines concentrations on a regional scale over the Yangtze River Delta region in east China. The WRF-Chem with nested grids is used in model simulations. In contrast to the very limited existing modeling studies that assumed a fixed ratio (FR) of amines to total ammonia emission, we derive source-dependent ratios (SDR) that distinguish C1-amine (CH 3 NH 2 ), C2-amines (C 2 H 7 N), C3-amines (C 3 H 9 N) emissions from five different source types (agriculture, residential, transportation, chemical industry, and other industry). The amines-to-ammonia mass emission ratios, estimated from previous measurements, are 0.026, 0.0015, 0.0011, 0.0011, and 0.0011 for C1-amine, 0.007, 0.0018, 0.0015, 0.01, and 0.0009 for C2-amines, and 0.0004, 0.0005, 0.00043, 0.0006, and 0.0004 for C3-amines for chemical-industrial, other industrial, agricultural, residential, and transportational sources, respectively. The simulated concentrations of C1-, C2-, and C3-amines, based on both FR and SDR, have been compared with field measurements at a suburban site in Nanjing and at an urban site in Shanghai, China. SDR substantially improves the model’s ability in capturing the observed concentrations of methylamines. C1-, C2-, and C3-amines concentrations in the surface layer in the Yangtze River Delta region are generally in the range of 2–20 pptv, 5–50 pptv, and 0.5–4 pptv. Vertically, the concentrations of C1-, C2-, and C3-amines decrease quickly with altitude, dropping by a factor of ~ 10 from the surface to ~ 900 hPa. Results from the present study are critical to evaluating potential roles of amines in nucleation and chemical processes in polluted air.