Inadequate air quality has adverse impacts on human well-being and contributes to the progression of climate change, leading to fluctuations in temperature. Therefore, gaining a localized comprehension of the interplay between climate variations and air pollution holds great significance in alleviating the health repercussions of air pollution. This study uses a holistic approach to make air quality predictions and multivariate modelling. It investigates the associations between meteorological factors, encompassing temperature, relative humidity, air pressure, and three particulate matter concentrations (PM10, PM2.5, and PM1), and the correlation between PM concentrations and noise levels, volatile organic compounds, and carbon dioxide emissions. Five hybrid machine learning models were employed to predict PM concentrations and then the Air Quality Index (AQI). Twelve PM sensors evenly distributed in Craiova City, Romania, provided the dataset for five months (22 September 2021–17 February 2022). The sensors transmitted data each minute. The prediction accuracy of the models was evaluated and the results revealed that, in general, the coefficient of determination (R2) values exceeded 0.96 (interval of confidence is 0.95) and, in most instances, approached 0.99. Relative humidity emerged as the least influential variable on PM concentrations, while the most accurate predictions were achieved by combining pressure with temperature. PM10 (less than 10 µm in diameter) concentrations exhibited a notable correlation with PM2.5 (less than 2.5 µm in diameter) concentrations and a moderate correlation with PM1 (less than 1 µm in diameter). Nevertheless, other findings indicated that PM concentrations were not strongly related to NOISE, CO2, and VOC, and these last variables should be combined with another meteorological variable to enhance the prediction accuracy. Ultimately, this study established novel relationships for predicting PM concentrations and AQI based on the most effective combinations of predictor variables identified.