This article is to depict the steps taken by our team for the development of glycosylated artificial metalloenzymes (GArMs) that we have used to develop therapeutic in vivo synthetic chemistry. To achieve this goal, we have had to combine technologies developed over the course of a decade that range from protein conjugation methodologies, identification of glycan-dependent targeting, development of functional biocatalysis, and biocompatible reactions. As a result, we have begun to reveal the framework for GArM complexes and their potential towards creating novel biotechnological tools and therapeutic applications.