Perfluorosulfonic acid (PFSA) dispersions are used as components in a variety of electrochemical technologies, particularly in fuel-cell catalyst-layer inks. In this study, we characterize dispersions of a common PFSA, Nafion, as well as inks of Nafion and carbon. It is shown that solvent choice affects a dispersion’s measured pH, which is found to scale linearly with Nafion loading. Dispersions in water-rich solvents are more acidic than those in propanol-rich solvents: a 90% water versus 30% water dispersion can have up to a 55% measured proton deviation. Furthermore, because electrostatic interactions are a function of pH, these differences affect how particles aggregate in solution. Despite having different water contents, all inks studied demonstrate the same particle size and surface charge trends as a function of pH, thus providing insights into the relative influence of solvent and pH effects on these properties.