Services are the fundamental to the provisioning of business activities. Enterprise Architecture (EA) is maintaining the relationship between strategy, business and technology. A clear definition and agreed understanding of services is critical to realising information technology artefacts. Services, however, tend to be more complex than the mere act of interaction or working process, and should be seen out of the cultural, organisational and managerial factors surrounding it. This chapter will use a service model consisting of execution, context and intention with an underlying claim that all three elements must be present to make services meaningful. EA must be seen in the light of this. This chapter addresses the issues related to organisational and system transition of services and subsequently EA when being transformed from loose, distributed organisations and into Shared Service Centres (SSCs). A case study is being presented where eGovernment services are moved from local government level and into a shared service centre structure. Major findings include (1) a model view relates services to actors, (2) an eGovernment services architecture maturity model, (3) a systemic and combinatorial approach to organising services architectures. This chapter aims at the deeper understanding of services in developing eGovernment architectures but findings are readily applicable in general business environments.