t The rapid increase and adoption of new Information Technologies (IT) in Smart Cities make the provision of public services more efficient. However, various municipalities and cities deal with challenges to transform and digitize city services. Smart Cities have a high degree of complexity where offered city services must respond to the concerns and goals of multiple stakeholders. These city services must also involve diverse data sources, multi-domain applications, and heterogeneous systems and technologies. Enterprise Architecture (EA) is an instrument to deal with complexity in both private and public organizations. The paper defines the concepts for modeling Smart Cities in ArchiMate, guided by a design-oriented research approach. Particularly, the focus of this paper is on the concepts for modeling city services and underlying information systems which are added to the EA metamodel. The metamodel is demonstrated in a real-world case and validated by Smart City domain experts. The findings suggest that these concepts are essential to achieve the Smart City strategy (e.g., city goals and objectives), as well as to meet the needs of different city stakeholders. Furthermore, an extension mechanism allows addressing the alignment of business and IT in complex environments such as Smart Cities, by adjusting EA metamodels and notations. This can help cities to design, visualize, and communicate architecture decisions when managing the transformation and digitalization of public services.