Mobile networks are highly complex systems. Therefore, it is crucial to examine them from an empirical perspective to better understand how network features affect performance, so to suggest additional improvements. To this aim, this paper presents a large-scale dataset of measurements collected over fourth generation (4G) and fifth generation (5G) operational networks, providing Long Term Evolution (LTE), Narrowband Internet of Things (NB-IoT), and 5G New Radio (NR) connectivity. We collected our dataset during seven weeks in Rome, Italy, by performing several tests on the infrastructures of two major mobile network operators (MNOs). The open-sourced dataset has enabled multi-faceted analyses of network deployment, coverage, and end-user performance, and can be further used for designing and testing artificial intelligence (AI) and machine learning (ML) solutions for network optimization.