Ambient air pollution has been associated with adverse neurological health outcomes. Ambient pollutants are thought to trigger oxidative stress and inflammation to which vulnerable populations, such as elderly may be particularly susceptible. Our study investigated the possible association between concentrations of ambient air pollutants and the number of emergency department (ED) visits for nervous system disorders among people residing in a large Canadian city. A time-stratified case-crossover study design combining data from the National Ambulatory Care Reporting System (NACRS) and the National Air Pollution Surveillance (NAPS) between 2004 and 2015 was used. Two air quality health indices were considered in additional to specific pollutants, including carbon monoxide (CO), nitrogen dioxide (NO2), sulfur dioxide (SO2), ozone (O3) and fine particulate matter (PM2.5). Weather condition data were included in the models. ED visits with a discharge diagnosis were identified using ICD-10 codes (G00-G99). The analysis was stratified by sex and age, also by seasons. The associations were investigated in arrays organized as 18 strata and 15 time lags (in days) for each pollutant. Overall, 140,511 ED visits were included for the analysis. Most ED visits were related to episodic and paroxysmal diagnoses (G40-G47, 64%), with a majority of visits for migraines (G43, 39%). Among females, an increase of 0.1ppm ambient CO was associated with an increased risk of paroxysmal diagnoses at day 1 (RR = 1.019 (95%CI 1.004-1.033)), day 6 (1.024 (1.010-1.039)) and day 7 (1.022 (1.007-1.036). PM2.5 and SO2, and air quality indices were similarly associated with ED visits for episodic and paroxysmal disorders in days 6 and 7. Findings highlight that ambient air pollution is associated with an increased number of ED visits for nervous system disorders, particularly visits for paroxysmal diagnoses.