Lake Superior is one of the largest freshwater lakes on our planet, but few optical observations have been made to allow for development and validation of visible spectral satellite remote sensing products. The dataset described here focuses on coincidently observing inherent and apparent optical properties along with biogeochemical parameters. Specifically, we observe remote sensing reflectance, absorption, scattering, backscattering, attenuation, chlorophyll concentration, and suspended particulate matter over the ice-free months of 2013–2016. The dataset substantially increases the optical knowledge of the lake. In addition to visible spectral satellite algorithm development, the dataset is valuable for characterizing the variable light field, particle, phytoplankton, and colored dissolved organic matter distributions, and helpful in food web and carbon cycle investigations, among others. The compiled data can be freely accessed at: https://seabass.gsfc.nasa.gov/archive/URI/Mouw/LakeSuperior/ .