Weakly Coordinated Cobaltacycles: Trapping Catalytically Competent Intermediates in Cp*CoIII Catalysis

Herein, we disclose the synthesis of metallacyclic Cp*Co III complexes containing weakly‐chelating functional groups. We have employed these compounds not only as an exceptional platform for accessing some of the most widely invoked transient intermediates in C–H functionalization processes but also as competent catalysts in different Cp*Co‐catalyzed transformations, including a benchmark coupling reaction.