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The definition of an Enterprise Architecture (EA) has a central role in implementing Information Systems (ISs) that proactively contribute to business and Information Technology (IT) alignment. In this paper, using a set of key concepts for the Information System Architecture (ISA) specification (formalized in a UML profile), 16 metrics are proposed for ISA suitability assessment considering a set of required quality characteristics. This paper also proposes an exploratory approach for the ISA definition process. This approach combines EA primitives and metrics in order to support multi-criteria ISA selection. The proposals presented in this research are applied in the definition, evaluation and comparing of different architectural options for the new Portuguese National identification document project (the Citizen Card project).