Aerosols are microscopic liquid or solid particles that enter the atmosphere through natural and man-made processes. Time series trends and correlations of aerosol optical depth and cloud parameters over Addis Ababa have become the subject of scientific research because of the importance of clouds in controlling climate. In this study, we have examined the temporal variations (time series analysis) in aerosol particles over Addis Ababa and the impact of these variations on various optical properties of clouds using Moderate Resolution Imaging Spectroradiometer (MODIS) data from January 2003 to December 2018. The maximum aerosol optical depth (AOD) was found during the summer period, with minimum values in winter. During summer, the air temperature is high, which leads to abundant atmospheric water vapor, facilitating the hygroscopic growth of aerosols. We then analyzed the relationships between AOD and other cloud parameters, namely, water vapor (WV), cloud fraction (CF), cloud top temperature (CTT), and cloud top pressure (CTP), to provide a better understanding of aerosol–cloud interactions. The correlation between AOD and CF and WV was positive for Addis Ababa, while there was a negative correlation with CTT and CTP.