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Abstract Studies of molecular mixtures containing hydrogen sulfide (H 2 S) could open up new routes towards hydrogen-rich high-temperature superconductors under pressure. H 2 S and ammonia (NH 3 ) form hydrogen-bonded molecular mixtures at ambient conditions, but their phase behavior and propensity towards mixing under pressure is not well understood. Here, we show stable phases in the H 2 S–NH 3 system under extreme pressure conditions to 4 Mbar from first-principles crystal structure prediction methods. We identify four stable compositions, two of which, (H 2 S) (NH 3 ) and (H 2 S) (NH 3 ) 4 , are stable in a sequence of structures to the Mbar regime. A re-entrant stabilization of (H 2 S) (NH 3 ) 4 above 300 GPa is driven by a marked reversal of sulfur-hydrogen chemistry. Several stable phases exhibit metallic character. Electron–phonon coupling calculations predict superconducting temperatures up to 50 K, in the Cmma phase of (H 2 S) (NH 3 ) at 150 GPa. The present findings shed light on how sulfur hydride bonding and superconductivity are affected in molecular mixtures. They also suggest a reservoir for hydrogen sulfide in the upper mantle regions of icy planets in a potentially metallic mixture, which couldmore »have implications for their magnetic field formation.« less