BACKGROUND: There is increasing interest in the health effects of air pollution. However, the relationships between ozone exposure and mortality attributable to neurological diseases remain unclear. OBJECTIVES: To assess associations of long-term exposure to ozone with death from Parkinson's disease, dementia, stroke, and multiple sclerosis. METHODS: Our analyses were based on the 2001 Canadian Census Health and Environment Cohort. Census participants were linked with vital statistics records through 2016, resulting in a cohort of 3.5 million adults/51,045,700 person-years, with 8,500/51,300/43,300/1,300 deaths from Parkinson's/dementia/stroke/multiple sclerosis, respectively. Ten-year average ozone concentrations estimated by chemical transport models and adjusted by ground measurements were assigned to subjects based on postal codes. Cox proportional hazards models were used to calculate hazard ratios (HRs) for deaths from the four neurological diseases, adjusting for eight common demographic and socioeconomic factors, seven environmental indexes, and six contextual covariates. RESULTS: The fully adjusted HRs for Parkinson's, dementia, stroke, and multiple sclerosis mortalities related to one interquartile range increase in ozone (10.1 ppb), were 1.09 (95% confidence interval 1.04-1.14), 1.08 (1.06-1.10), 1.06 (1.04-1.09), and 1.35 (1.20-1.51), respectively. The covariates did not influence significance of the ozone-mortality associations, except airshed (i.e., broad region of Canada). During the period of 2001-2016, 5.66%/5.01%/ 3.77%/19.11% of deaths from Parkinson's/dementia/stroke/multiple sclerosis, respectively, were attributable to ozone exposure. CONCLUSIONS: We found positive associations between ozone exposure and mortality due to Parkinson's, dementia, stroke, and multiple sclerosis.