Smoke from forest fires contains significant amounts of gaseous and particulate pollutants. Firefighters exposed to wildland fire smoke can suffer from several acute and chronic adverse health effects. Consequently, exposure data are of vital importance for the establishment of cause/effect relationships between exposure to smoke and firefighter health effects. The aims of this study were to (1) characterize the relationship between wildland smoke exposure and medical parameters and (2) identify health effects pertinent to wildland forest fire smoke exposure. In this study, firefighter exposure levels of carbon monoxide (CO), nitrogen dioxide (NO₂), and volatile organic compounds (VOC) were measured in wildfires during three fire seasons in Portugal. Personal monitoring devices were used to measure exposure. Firefighters were also tested for exhaled nitric oxide (eNO) and CO before and after their firefighting activities. Data indicated that exposure levels during firefighting activities were beyond limits recommended by the Occupational Exposure Standard (OES) values. Medical tests conducted on the firefighters also indicated a considerable effect on measured medical parameters, with a significant increase in CO and decrease in NO in exhaled air of majority of the firefighters.