Cobalt arsenide deposits associated with Neoproterozoic serpentinite in Morocco represent the highest-grade cobalt resource worldwide. Yet, genetic models for their origin remain controversial. We report here mineralogical and geochemical evidence for arsenide-calcite mineralization at Bou Azzer to constrain the temporal framework and identify the geodynamic trigger for mineralization mechanisms. To this end, radiometric ages for ore minerals are paramount for understanding the origin of the Bou Azzer cobalt arsenide deposit. New safflorite (CoAs2) rhenium-osmium (Re-Os) ages are Late Devonian in age: 380.4 ± 2.9 and 373.4 ± 1.2 to 368.1 ± 5.0 million years ago (Ma) for coarse-grained and fine-grained safflorite, respectively. These dates overlap with the timing of break-up of the supercontinent Gondwana, and the building of an arch-and-basin geometry from northern Africa to Arabia. Our findings temporally and spatially contextualize previous knowledge of fluid chemistry and mineralization mechanisms involving a two-fluid mixing. Arsenide mineralization resulted from mixing of a methane-dominated fluid with highly saline basinal brines that leached Os (187Os/188Osinitial = 0.120 ± 0.001), and by corollary cobalt, from Neoproterozoic serpentinite. Carbon and sulfur stable isotope data of ore-stage calcite and arsenides, respectively, show that hydrocarbons acted as the main reductant for mineralization. We speculate that the seawater-derived brines sank into the sedimentary basins adjacent to a carbonate platform with the Bou Azzer serpentinite in its basement in the Late Devonian. In the context of an enhanced geothermal gradient, such brines would have been involved in warm hydrothermal alteration of hydrocarbon source rocks of the local expression of the Kellwasser event in the geological record of present-day Morocco. This warm hydrothermal alteration of hydrocarbon source rocks may have taken place for coarse-grained safflorite mineralization (380.4 ± 2.9 Ma) shortly after ca. 382–381 Ma Lower Kellwasser horizons were deposited, or, for fine-grained safflorite mineralization (373.4 ± 1.2 to 368.1 ± 5.0 Ma) while the Upper Kellwasser horizons of present-day Morocco were being deposited.