A large dataset for PM2.5 and PMcoarse (PM2.5-10) concentrations monitored near a busy London highway (Marylebone Road) has been analyzed to define the factors that lead to high concentrations. The following have been highlighted as major influencing parameters: wind speed, prevailing wind direction (because of its role on the microscale dispersion within the street), the daily cycle of the atmospheric boundary layer (stable during the night/ convective and mixed during the day), and traffic density. The mainly diesel heavy-duty vehicles are the main source of fine particulate matter at Marylebone Road. In particular, lorries (trucks) dominate PM10 exhaust emissions which are mainly in the fine (<2.5 microm) size range. A strong correlation with PMcoarse suggests that the heavy-duty traffic is largely responsible for this component also. Substantial local increments in PM2.5 and PMcoarse due to traffic have been estimated and a large part of the increment in PMcoarse concentrations is inferred to arise from resuspended road dust emissions since the contribution of abrasion processes estimated from emission factors is modest. Despite the strong influence of traffic on PM concentrations measured at Marylebone Road the analysis of factors leading to the highest 5% of hourly concentrations of PM10 at Marylebone Road reveals that almost half of these events were due to building works. The other events occurred when all or most of the key factors occurred simultaneously (heavy traffic, poor dispersion, etc.). Some episodes of high PM2.5 concentrations were associated with long-range transport in which the regional PM2.5 constituted most of the local concentrations.