Phosphate minerals play an important role in the natural cycle of phosphorous, both in the solid form used in agricultural applications and as aerosolized apatite mineral particles. Mineral surface aging processes, such as organic acid processing, have a significant effect on the phosphate particle physicochemical properties, particularly, their hygroscopicity. In this study, hydroxyapatite was used as a model for low solubility apatite phosphate minerals and subjected to acid processing with formic acid (FA) vapor to simulate the atmospheric processing caused by volatile organic compounds present in the troposphere. Hydroxyapatite particles were shown to react with the FA vapor to form Ca(HCOO) 2 on the particle surface, resulting in a heterogeneous microparticle surface, as evidenced by spatially resolved Raman spectroscopy. Due to the more soluble nature of the Ca(HCOO) 2 formed on the surface, the hygroscopicity of the acid-processed particle surfaces was shown to increase using dynamic vapor sorption studies. The maximum water uptake at 95% RH was shown to increase from 0.4 to 0.82% and 3.26% after 24 and 48 h of laboratory acid exposure, respectively. Conventional adsorption models, including Brunauer−Emmett−Teller and Freundlich, were used to fit the adsorption data. The heat of sorption values of the 48 h acid-exposed sample was shown to converge to the heat of condensation of water at higher coverage values compared to untreated and 24 h processed hydroxyapatite.