Multimodal datasets of materials are rich sources of information which can be leveraged for expedited discovery of process-structure-property relationships and for designing materials with specific structures and/or properties. Here, we provide a multimodal dataset of magnetron sputter-deposited molybdenum (Mo) thin films, which are used in a variety of industries including high temperature applications, photovoltaics, and microelectronics. A process space consisting of 27 unique combinations of sputter power and Argon (Ar) deposition pressure was explored. The structure and surface morphology of the Mo thin films was characterized by X-ray diffraction, atomic force microscopy, and scanning electron microscopy. Physical properties – namely, residual stress and resistivity – were also measured to provide additional film characteristics and behaviors. The entire dataset consists of 1377 measurements including scalar values (e.g. residual stress values), 2D linescans (e.g. X-ray diffractograms), and 3D imagery (e.g. atomic force microscopy images). We acknowledge the Laboratory Directed Research and Development program forproviding funding for this study. This work was performed, in part, at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA0003525. The views expressed in the article do not necessarily represent the view of the U.S. DOE or the United States Government.