A new validation campaign was conducted at the W2 Harold Alfond Ocean Engineering Laboratory at the University of Maine to investigate the hydrodynamic loading on floating offshore wind substructures, with a focus on the low-frequency contributions that tend to drive extreme and fatigue loading in semisubmersible designs. A component-level approach was taken to examine the hydrodynamic loads on individual parts of the semisubmersible in isolation and then in the presence of other members to assess the change in hydrodynamic loading. A variety of wave conditions were investigated, including bichromatic waves, to provide a direct assessment of difference-frequency wave loading. An assessment of the impact of wave uncertainty on the loading was performed, with the goal of enabling validation with this dataset of numerical models with different levels of fidelity. The dataset is openly available for public use and can be downloaded from the U.S. Department of Energy Data Archive and Portal.