Samples of FeS were oxidized by oxygen-bearing acidic solutions at 25• C and different initial pH values (2.75 ≤ pH ≤ 3.45). The reacted FeS samples were investigated by scanning electron microscopy (SEM), nitrogen adsorption/desorption isotherms measurements, and FT-Raman spectroscopy. A sulfur rich phase (layer) is inferred to be form on reacting FeS surface based on sequential extraction with acidic chromium(II) chloride solutions. The sulfur-rich layer (SRL) formed on oxidized FeS samples is traversed by various mesopores with average pore size <450Å. It is reasonable to assume that the mesopores facilitate the migration of iron and sulfur from FeS structure into solution across SRL. The FT-Raman spectra of oxidized FeS samples show an intense peak at 162 cm −1 , which can be attributed to SRL developed on FeS surface. A model for SRL development on FeS during its oxidation by dissolved oxygen has been proposed from the present results and previous studies.