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. We include an extensive set of eight experimental characterization modalities for each unique power/pressure combination: X-ray diffraction, scanning electron microscopy, residual stress, resistivity, atomic force microscopy, rutherford backscattering, nanoindentation, and transmission electron microscopy with automated crystal orientation mapping data. We also include simulated experiments over an expanded set of powers, pressures and working distances to capture process data in addition to this experimental structure and property data. We acknowledge the Laboratory Directed Research and Development program for providing 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.