Air pollution is a serious problem in Romania, with the country ranking 13th among the most polluted countries in Europe in the 2021 World Air Quality Report. Despite the recognized impact of pollutants on health, there has been a lack of large-scale studies conducted in Romania. This study investigated the impact of air pollutants on patients with chronic respiratory, cardiovascular, cerebrovascular, or metabolic diseases in Bucharest and its metropolitan area from 20 August 2018 to 1 June 2022. The daily limit values for particulate matter PM10 and PM2.5 were exceeded every month, especially during the cold season, with a decrease during the COVID-19 pandemic restrictions. A significant statistical correlation was found between the monthly average values of PM2.5 and PM10 and hospitalizations for respiratory and cardiovascular diseases. A 10 µg/m³ increase in monthly average values resulted in a 40–60% increase in admissions for each type of pathology, translating to more than 2000 admissions for each pathology for the study period. This study highlights the urgent need for national and local measures to ensure a cleaner environment and enhance public health in Romania according to international regulations.