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Urban air pollution has emerged as a prominent public health concern in megacities and highly developed city clusters. Accurate modelling of urban air quality over complex terrain is challenging due to heterogeneous urban landscapes and multiscale land-atmosphere interactions. In this study, we investigated the applicability of urban canopy models in the Weather Research and Forecast (WRF) model and assessed the impacts of implementing these models on the urban air quality simulation in the Community Multiscale Air Quality (CMAQ) model over the megacity Chengdu, southwestern China. The land use and land cover of Chengdu were updated in WRF by using the land-use products in 2017 from the Moderate-resolution Imaging Spectroradiometer (MODIS). Sensitivity experiments with various urban canopy models were conducted to investigate the feasibility of different urban canopy models on WRF-CMAQ simulations. We found that the SLAB model significantly underestimates NO2 and PM2.5 concentrations, with mean fractional bias in winter (summer) reaching 52.93% (−50.34%) and −102.82% (−23.12%), respectively. Such large biases are mainly attributed to overpredicted wind speeds resulting from the flat structure in the SLAB model. In contrast, the BEM (a multilayer urban canopy model coupled with air-conditioning systems) model yields the best model performance in both winter and summer, with mean fractional errors of 33.15% (38.96%) and 34.10% (33.15%) for NO2 and PM2.5 in winter (summer), respectively. The UCM (a single-layer urban canopy model) model illustrates good performance in summer, with MFBs of 25.61% for NO2 and 19.03% for PM2.5, while NO2 and PM2.5 concentrations are overestimated in winter, with MFBs of 62.58% and 38.19%, respectively. In contrast, BEP (a multilevel urban canopy model)-modelled NO2 (MFB: 37.18%) and PM2.5 (MFB: 18.72%) correlate well with observations in winter, while significantly overestimated air pollutant concentrations in summer with MFBs of NO2 and PM2.5 of 49.70% and 44.50%, respectively. In general, the BEP model and the BEM model are well suited for air quality simulations over Chengdu in winter, and the BEM model could be considered for air quality simulations in summer. Furthermore, we assessed the effects of extensive usage of air conditioning systems in Chengdu during summertime, and the results suggest that using air conditioning systems facilitates the dispersion of air pollutants over Chengdu. This study pinpoints the limitations of default WRF configurations and tests the applicability of urban canopy models in the WRF-CMAQ model over Chengdu, in addition highlighting the crucial role of urban canopy models in urban meteorological-air quality simulations. 1. The feasibility of different urban canopy models in complex terrain is investigated over the megacity Chengdu. 2. Overestimation of wind speed under weak wind fields has been improved by employing urban canopy models. 3. The extensive use of air conditioning systems shows improvements in air quality over Chengdu in summer. [ABSTRACT FROM AUTHOR]