Air pollution causes premature mortality and morbidity globally, but these adverse health effects occur over proportionately in low- and middle-income countries. Lack of both air pollution data and knowledge of its spatial distribution in African countries have been suggested to lead to an underestimation of health effects from air pollution. This study aims to measure nitrogen oxides (NOx), as well as nitrogen dioxide (NO2), to develop Land Use Regression (LUR) models in the city of Adama, Ethiopia. NOx and NO2 was measured at over 40 sites during six days in both the wet and dry seasons. Throughout the city, measured mean levels of NOx and NO2 were 29.0 µg/m3 and 13.1 µg/m3, respectively. The developed LUR models explained 68% of the NOx variances and 75% of the NO2. Both models included similar geographical predictor variables (related to roads, industries, and transportation administration areas) as those included in prior LUR models. The models were validated by using leave-one-out cross-validation and tested for spatial autocorrelation and multicollinearity. The performance of the models was good, and they are feasible to use to predict variance in annual average NOx and NO2 concentrations. The models developed will be used in future epidemiological and health impact assessment studies. Such studies may potentially support mitigation action and improve public health.