This case study describes how librarians and enterprise architects at an Australian university worked together to document key components of the Library’s “as-is” enterprise architecture (EA). The article covers the rationale for conducting this activity, how work was scoped, the processes used, and the outputs delivered. The author discusses the short-term benefits of undertaking this work, with practical examples of how outputs from this process are being used to better plan future library system replacements, upgrades, and enhancements. Longer-term benefits may also accrue in the future as the results of this architecture work inform the Library’s IT planning and strategic procurement. This article has implications for practice for library technology specialists as it validates views from other practitioners on the benefits for libraries in adopting enterprise architecture methods and for librarians in working alongside enterprise architects within their organizations.