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Few studies have investigated the relationship between ambient air pollution and cardiorespiratory outcomes in Africa. A cross-sectional study comprising of 572 adults from four informal settlements in the Western Cape, South Africa was conducted. Participants completed a questionnaire adapted from the European Community Respiratory Health Survey, and the National Health and Nutrition Examination Survey questionnaire. Exposure estimates were previously modelled using Land-Use Regression for Particulate Matter (PM2.5) and Nitrogen Dioxide (NO2) at participants' homes. The median age of the participants was 40.7 years, and 88.5% were female. The median annual NO2 level was 19.7 microg/m(3) (interquartile range [IQR: 9.6-23.7]) and the median annual PM2.5 level was 9.7 microg/m(3) (IQR: 7.3-12.4). Logistic regression analysis was used to assess associations between outcome variables and air pollutants. An interquartile range increase of 5.12 microg/m(3) in PM2.5 was significantly associated with an increased prevalence of self-reported chest-pain, [Odds ratio: 1.38 (95% CI: 1.06-1.80)], adjusting for NO2, and other covariates. The study found preliminary circumstantial evidence of an association between annual ambient PM2.5 exposure and self-reported chest-pain (a crude proxy of angina-related pain), even at levels below the South African National Ambient Air Quality Standards.