Relational coordination suggests that high-quality relationships improve coordination. Yet as the landscape of work shifts toward digitization of coordination processes, organizations increasingly rely on digitally mediated structured coordination to accomplish work, reducing opportunities for personal interactions. In this article we explore the interplay between employees' work relationships and differently structured coordination mechanisms to theorize about the role of relational coordination in coordination that is becoming increasingly structured owing to digitization. Specifically, we identify four categories of coordination mechanisms by leveraging two distinct components of a coordination mechanism-actor selection and content delivery-and recognizing that either component can be structured or unstructured. This granular categorization of coordination mechanisms allows us to delineate three causal routes by which relational coordination adds value to coordination enactment: informing actor selection, informing customization of content, and enabling shared interpretation. We complement prior research focusing on how, over time, coordination mechanisms influence the development of relational coordination by theorizing about how relational coordination enables the effective enactment of coordination mechanisms at a point in time. Our findings complement the understanding of the interplay between relational coordination and coordination mechanisms and can inform the design of coordination mechanisms in digitized work processes.