The Rocabruna and Coll de Pal barite deposits, located in the eastern Pyrenees of Spain, fill karstic cavities within carbonate rocks of Cambrian and Devonian age, respectively. The deposits contain barite, chalcopyrite, tetrahedrite, pyrite and minor sphalerite and galena with saddle dolomite and quartz as gangue. Fluid inclusion data from Coll de Pal quartz and dolomite indicate that the mineralizing fluid was a polysaline CaCl2-rich brine, with temperatures between 125 and 150 °C. C and O isotopic compositions of carbonates in both deposits are consistent with a progressive increase in temperature during deposition. The δ34S values of barite, which range from 14.2 to 15.9‰ in Coll de Pal, and from 13.9 to 19.3‰ in Rocabruna, together with 87Sr/86Sr ratios ranging from 0.7118 to 0.7168 in Rocabruna, and from 0.7115 to 0.7136 in Coll de Pal, indicate two different fluid sources. We propose that these deposits formed as a result of mixing between a Ba-rich, sulfate-poor hot fluid, and sulfate-rich solutions of surficial origin. The different Sr isotope ratios in the deposits indicate that the hot Ba-rich fluids involved in each deposit were equilibrated with different rock types (carbonates and shales), in agreement with the geology of the two areas.