The equilibrium thermodynamics of Fe/Mg-phyllosilicates and carbonates have been investigated using numerical modeling, with emphasis on the effects of evaporation and temperature (hydrothermalism) under conditions related to present-day and primitive Mars, that is, low or high CO 2 partial pressure, under oxidizing or reducing environments. Findings are discussed in relation to alteration and weathering of minerals found in the Nili Fossae region. Results show that nontronite precipitates at very high water-to-precipitate ratio and low temperature, in association with ferrihydrite. During evaporation, this assemblage leads to carbonates: calcite and magnesite, and to low temperature iron-rich serpentine phyllosilicates such as cronstedtite or berthierine under reducing conditions. At high temperature, the initial paragenesis dominated by nontronite leads to hematite and berthierine at low CO 2 partial pressure, and to talc, magnesite and antigorite at high CO 2 partial pressure. Thus, the Fe/Mg-smectites, Mg-carbonate, and Mg-serpentine found near Nili Fossae may result from several alteration events. Weathering of primitive bedrock formed nontronite, with subsequent or concurrent hydrothermalism leading to Mg-serpentine. Further carbonation due to CO 2 -rich fluids led to talc, magnesite and to hydrogen/carbon monoxide/methane in the presence of iron, but at relatively low partial pressures (up to 10 −4 bar). Unless the serpentinization process acted for extended periods of time and over a large portion of the martian surface, it is unlikely it significantly contributed to the atmospheric composition, except maybe for H 2 . However, such water-rich active environments with the presence of redox reactions could have been suitable for the potential emergence of biological activity.Plain Language Summary Multiple locations on Mars exhibit phyllosilicate deposits, which have been used as indicators of temperate paleoenvironments with abundant liquid water. Of these, Nili Fossae is one of the rare occurrences where additional phases such as carbonates or serpentine are found. These minerals also pinpoint to possible hydrothermal activity, which is very important for the putative emergence of biologic activity on the red planet. Our work aims at understanding these various environments using numerical thermodynamic simulations of the mineral assemblages observed in this province. We observe that Mg,Fe-phyllosilicates such as nontronite form in low temperatures environments with very abundant water, and relatively oxidizing conditions (so rather on the surface) while magnesite and serpentine mixtures are characterized by higher temperatures (typically 200-300 °C) in the presence of high CO 2 partial pressures and more reducing conditions. Such hydrothermal reactions should also have led to the formations of hydrogen, carbon monoxide, and perhaps methane, but at concentrations probably too low to allow for global warming on Mars, unless they would have been significantly extended geographically and temporally. Nonethel...