This study systematically examines how the urban heat island (UHI) and urban breeze circulation (UBC) respond to an increase in roof albedo (αr) and its influence on urban air pollutant dispersion. For this, idealized ensemble simulations are performed using the Weather Research and Forecasting (WRF) model. The increase in αr from 0.20 to 0.65 decreases the UHI intensity, UBC intensity, and urban planetary boundary layer (PBL) height in the daytime (from 1200 to 1700 LST) by 47%, 36%, and 6%, respectively. As both UBC intensity and urban PBL height decrease, the daytime urban near-surface passive tracer concentration increases by 115%. The daytime UHI intensity, UBC intensity, and urban tracer concentration nonlinearly change with αr: For 0.10 ≤ αr < 0.80, the rates of changes in the UHI intensity, UBC intensity, and urban tracer concentration with αr overall increase as αr increases. For αr ≥ 0.80, the daytime roof surface temperature is notably lower than the daytime urban near-surface air temperature, the UHI intensity, UBC intensity, and urban tracer concentration very slightly changing with αr. This study provides insights into the associations between changes in roof surface temperature and roof surface energy fluxes with αr and those in UHI intensity.