Recent epidemiologic studies have shown an association between low serum folate levels and risk of vascular disease, including stroke and various types of vascular cognitive impairment. We examined data from the Canadian Study of Health and Aging (CSHA), a population-based, prospective 5-year investigation of the epidemiology of dementia among Canadians aged 65+ years. The risk of an adverse cerebrovascular event (including vascular dementia, vascular cognitive impairment, or fatal stroke) during follow-up, was assessed according to serum folate quartiles among subjects with no evidence of dementia at baseline (n = 369). After adjusting for certain covariates, including cardiovascular disease and nutritional indices, education, smoking and baseline cognitive status, the risk estimate for an adverse cerebrovascular event associated with the lowest folate quartile compared with the highest quartile was OR 2.42 (95% CI 1.04–5.61). Results from stratified analyses also showed that relatively low serum folate was associated with a significantly higher risk of an adverse cerebrovascular event among female (OR 4.02, 95% CI 1.37–11.81) but not male (OR 1.02, 95% CI 0.25–4.13) subjects. Among the total sample, there was a consistent trend toward poorer health and cognitive outcomes during follow-up (including mortality, cognitive decline and dementia) among those in the lowest folate quartile compared with the highest quartile. Low serum folate levels are independently associated with a significantly higher risk of an adverse cerebrovascular event, including vascular dementia and stroke death, among older, cognitively vulnerable persons.