The concept of “Smart Cities,” widely adopted in recent years globally, attempts to provide solutions to many urban challenges. The multiple challenges faced by modern cities globally, driven by continuous urbanization combined with other critical issues confronting the planet, are leading to the adoption of policies based on sustainable development and the opportunities offered by Information and Communication Technologies (ICT). Achieving a high standard of living and citizen welfare is central to urban governance. Examples of cities at both national and international levels are presented, along with innovative initiatives aimed at enhancing quality of life. Greek cities have similarly begun moving towards this model. This research paper analyzes the concept and characteristics of Smart Cities, as well as their significance. Within the framework of this study, a structured quantitative survey was conducted in the Municipality of Larissa, Greece, targeting a convenient sample of 141 residents. The survey examined citizens’ awareness, use, and perception of digital services and smart city initiatives implemented by the municipality. The findings show that, although citizens recognize the benefits of using ICTs, they remain in a transitional stage, displaying limited familiarity with digital services and a low degree of participation in decision-making processes. In summary, the results contribute to the ongoing discourse on smart governance and the crucial role of citizens in its overall success. Beneficiaries of the study include municipal authorities, urban planners, technology providers, and policymakers aiming to improve quality of life through smart and inclusive urban strategies.