Monthly average ambient concentrations of gaseous nitric acid (HNO3) and ammonia (NH3) were monitored at the Athabasca Oils Sands Region (AOSR), Alberta, Canada, between May 2005 and September 2008. Generally, concentrations of both pollutants were elevated and highly variable in space and time. The highest atmospheric concentrations occurred in the vicinity of the major mining and oil extraction activities of Fort Murray and Fort McKay. Maximum monthly average concentrations of HNO3 decreased from >6 μg m–3 2005 and 2006 to <4 μg m–3 in 2007 and 2008. While the HNO3 summer seasonal averages in 2005 and 2006 approached ~2 μg m–3 at some sites, in the subsequent summers and during winter seasons it rarely exceeded 1 μg m–3 and no clear differences between summer and winter occurred. Concentrations of NH3 were elevated during the entire study and frequently reached 6 μg m–3. Generally, NH3 stayed higher in summer than in winter; the summer seasonal averages often exceeded 4 μg m–3 while those for winter only on two occasions were above 3 μg m–3. In summer 2008, an expansion of the area with elevated NH3 levels was observed extending to remote locations. Ammonia is of a much higher concern from a perspective of possible biological effects, because of its potential for direct toxic effect on lichens and its contribution to the elevated N dry deposition with possible negative consequences for forests and other ecosystems.