The development, characterization, and exploitation of novel materials based on the assembly of molecular components is an exceptionally active and rapidly expanding field. For this reason, the topic of molecule-based materials (MBMs) was chosen as the subject of a workshop sponsored by the Chemical Sciences Division of the United States Department of Energy. The purpose of the workshop was to review and discuss the diverse research trajectories in the field from a chemical perspective, and to focus on the critical elements that are likely to be essential for rapid progress. The MBMs discussed encompass a diverse set of compositions and structures, including clusters, supramolecular assemblies, and assemblies incorporating biomolecule-based components. A full range of potentially interesting materials properties, including electronic, magnetic, optical, structural, mechanical, and chemical characteristics were considered. Key themes of the workshop included synthesis of novel components, structural control, characterization of structure and properties, and the development of underlying principles and models. MBMs, defined as "useful substances prepared from molecules or molecular ions that maintain aspects of the parent molecular framework" are of special significance because of the capacity for diversity in composition, structure, and properties, both chemical and physical. Key attributes are the ability in MBMs to access the additional dimension of multiple length scales and available structural complexity via organic chemistry synthetic methodologies and the innovative assembly of such diverse components. The interaction among the assembled components can thus lead to unique behavior. A consequence of the complexity is the need for a multiplicity of both existing and new tools for materials synthesis, assembly, characterization, and theoretical analysis. For some technologically useful properties, e.g., ferro- or ferrimagnetism and superconductivity, the property is not a property of a molecule or ion; it is a cooperative solid-state (bulk) property-a property of the entire solid. Hence, the desired properties are a consequence of the interactions between the molecules or ions, and understanding the solid-state structure as well as methods to predict, control, and modulate the structure are essential to understanding and manipulating such behaviors. As challenging as this is, molecules enable a substantially greater ability of control than atoms as building blocks for new materials and thus are well positioned to contribute significantly to new materials. The diversity of components and processes leads to the recognition of the critical role of cross-disciplinary research, including not only that between traditionally different areas within chemistry, but also between chemistry and biochemistry, physics, and a number of engineering disciplines. Enhancing communication and active collaboration between these groups was seen as a critical goal for the research area.