Despite the societal and economic impacts of the COVID-19 pandemic, the lockdown measures put in place by the Italian government provided an unprecedented opportunity to increase our knowledge of the effect transportation and industry-related emissions have on the air quality in our cities. This study assessed the effect of reduced emissions during the lockdown period, due to COVID-19, on air quality in three Italian cities, Florence, Pisa, and Lucca. For this study, we compared the concentration of particulate matter PM10, PM2.5, NO2, and O3 measured during the lockdown period, with values obtained in the same period of 2019. Our results show no evidence of a direct relationship between the lockdown measures implemented and PM reduction in urban centers, except in areas with heavy traffic. Consistent with recently published studies, we did, however, observe a significant decrease in NO2 concentrations among all the air-monitoring stations for each city in this study. Finally, O3 levels remained unchanged during the lockdown period. Of note, there were slight variations in the meteorological conditions for the same periods of different years. Our results suggest a need for further studies on the impact of vehicular traffic and industrial activities on PM air pollution, including adopting holistic source-control measures for improved air quality in urban environments.