Sulfates are abundant at the Martian surface, incorporating sulfur delivered by volcanic eruptions and degassing. The thickest sulfate accumulations are found in the interior layered deposits (ILDs) of Valles Marineris. The ILDs have been interpreted as either purely sedimentary deposits or weathered volcanic products. We performed nonlinear spectral unmixing of CRISM data located in the lower, massive member of the ILD pile in Ophir Chasma. The best spectral fit is obtained when primary igneous minerals (orthopyroxene, plagioclase) and coquimbite were present, alongside kieserite and szomolnokite, which were identified in previous ILD studies. Geomorphological evidence shows that the igneous minerals are from a source within the ILDs. Our findings suggest that the deposition of the lower member of the ILDs was influenced by Tharsis-related syntectonic and synvolcanic activity within the subsided Valles Marineris plateau, and by the redox state of an overlying Valles Marineris sea in a geologic context akin to volcanogenic massive sulfide deposition on Earth. Subsequent climate cooling, potentially related to Tharsis activity waning, would have led to gradual sea freezing, resulting in further alteration in acid-cold environment, and precipitation of the polyhydrated sulfates that compose the upper, layered ILD member. ILD erosion by glacial flows down to the currently exposed chasma floor level and aeolian erosion have shaped the current ILD morphology. In summary, the comprehensive ILD pile formed by in-situ weathering of volcanic products, redox state instabilities, and water level fluctuations in a warming and cooling Valles Marineris sea.