The concentration of surface ozone (O3) strongly depends on environmental and meteorological variables through a series of complex and non-linear functions. This study aims to explore the performances of an advanced machine learning (ML) method, the boosted regression trees (BRT) technique, in exploring the relationships between surface O3 and its driving factors, and in predicting the levels of O3 concentrations. To this end, a BRT model was trained on hourly data of air pollutants and meteorological parameters, acquired, over the 2016–2018 period, in a rural area affected by an anthropic source of air pollutants. The abilities of the BRT model in ranking, visualizing, and predicting the relationship between ground-level O3 concentrations and its driving factors were analyzed and illustrated. A comparison with a multiple linear regression (MLR) model was performed based on several statistical indicators. The results obtained indicated that the BRT model was able to account for 81% of changes in O3 concentrations; it slightly outperforms the MLR model in terms of the predictions accuracy and allows a better identification of the main factors influencing O3 variability on a local scale. This knowledge is expected to be useful in defining effective measures to prevent and/or mitigate the health damages associated with O3 exposure.