Air pollution can cause many adverse health outcomes, including cardiovascular and respiratory disorders. Land use regression (LUR) models are frequently used to describe small-scale spatial variation in air pollution levels based on measurements and geographical predictors. They are particularly suitable in resource limited settings and can help to inform communities, industries, and policy makers. Weekly measurements of NO2 and PM2.5 were performed in three informal areas of the Western Cape in the warm and cold seasons 2015–2016. Seasonal means were calculated using routinely monitored pollution data. Six LUR models were developed (four seasonal and two annual) using a supervised stepwise land-use-regression method. The models were validated using leave-one-out-cross-validation and tested for spatial autocorrelation. Annual measured mean NO2 and PM2.5 were 22.1 μg/m3 and 10.2 μg/m3, respectively. The NO2 models for the warm season, cold season, and overall year explained 62%, 77%, and 76% of the variance (R2). The PM2.5 annual models had lower explanatory power (R2 = 0.36, 0.29, and 0.29). The best predictors for NO2 were traffic related variables (major roads, bus routes). Local sources such as grills and waste burning sites appeared to be good predictors for PM2.5, together with population density. This study demonstrates that land-use-regression modelling for NO2 can be successfully applied to informal peri-urban settlements in South Africa using similar predictor variables to those performed in Europe and North America. Explanatory power for PM2.5 models is lower due to lower spatial variability and the possible impact of local transient sources. The study was able to provide NO2 and PM2.5 seasonal exposure estimates and maps for further health studies.