This tutorial review details the emergence of template-directed synthesis of metal-organic materials (MOMs) with emphasis upon reports of MOMs in which the template is retained, template@MOMs, and structurally characterized. Such MOMs enable analysis of the nature of the intermolecular interactions that occur between the template and the resulting host framework. The utilization of such understanding can enable template-directed synthesis to serve as a crystal engineering tool for the preparation of new MOMs, especially those that cannot be accessed without the use of a template. We anticipate that this review will guide future research by delineating several rules for identifying appropriate templates and molecular building blocks to afford MOMs with targeted structures and properties.