In today’s rapidly urbanizing world, the surge in urban population has led to height-ened transportation demands and intricate mobility patterns. However, the pursuit of efficient mobility must not compromise the safety of Vulnerable Road Users, including pedestrians, cyclists, children, elderly individuals, and those with disabilities [17,18]. The “Predictive Approaches for Safer Urban Environment” (PHOEBE) project addresses this pressing concern by employing predictive techniques to enhance safety measures for Vulnerable Road Users. This study not only focuses on investigating parameters influencing pedestrian, cyclist, and scooter movements in the center of Athens, but also examines the temporal variations in these movements and the impact of urban mobility interventions. Three Multiple Linear Regression Models were deployed, with the number of pedestrians, cyclists and scooters as dependent variables. Field measurements data were collected before and after the implementation of interventions under the Athens Great Walk framework. This dual approach allows for a comprehensive analysis of how VRU volumes vary by weekday, month, and hour of the day. The results underscore the positive impact of Athens Great Walk: reducing traffic lanes and expanding sidewalks led to significant increases in pedestrian and cyclist numbers. Sub-sequent interventions increase road user counts. Road type, traffic lanes, and pavement width were identified as statistically significant factors contributing to the rise in vulnerable users. These findings offer valuable guidance for policymakers and stakeholders striving to create secure environments for road users, forming a crucial foundation for pedestrian-friendly urban spaces. This research not only fills a crucial gap in under-standing urban transformation in metropolitan areas but also provides practical insights for promoting cycling as a viable transport mode in Athens, aligning with the global shift toward sustainable urban mobility.