These are discrete observations of total dissolved inorganic carbon (DIC) and alkalinity (TA), and associated computed CO2-system parameters, from samples collected throughout the Chesapeake Bay mainstem between 2016 and 2018. Samples were collected on board the R/V Kerhin in Maryland and the R/V Fay Slover in Virginia at a subset of fixed stations in collaboration with the Chesapeake Bay Water Quality Monitoring Program. Samples were analyzed following standard procedures at the Virginia Institute of Marine Science. The DIC and TA data were then used to compute the remaining CO2-system parameters (pH, CO2 partial pressure (pCO2), and carbonate saturation state). A detailed description of sample collection and analytical methods is given Friedman et al., 2019