We report new petrological, phase equilibria modeling, and fluid inclusion data for pelitic and mafic granulites from Rundvågshetta in the highest-grade region of the Neoproterozoic Lützow-Holm Complex (LHC), East Antarctica, and provide unequivocal evidence for fluid-rock interaction and high-temperature metasomatism in the presence of brine fluid. The studied locality is composed dominantly of well-foliated pelitic granulite (K-feldspar + quartz + sillimanite + garnet + ilmenite) with foliation-parallel bands and/or layers of mafic granulite (plagioclase + orthopyroxene + garnet + ilmenite + quartz + biotite). The boundary between the two lithologies is defined by thin (about 1–20 cm in thick) garnet-rich layers with a common mineral assemblage of garnet + plagioclase + quartz + ilmenite + biotite ± orthopyroxene. Systematic increase of grossular and decrease of pyrope contents in garnet as well as decreasing Mg/(Fe + Mg) ratio of biotite from the pelitic granulite to garnet-rich rock and mafic granulite suggest that the garnet-rich layer was formed by metasomatic interaction between the two granulite lithologies. Phase equilibria modeling in the system NCKFMASHTO demonstrates that the metasomatism took place at 850–860 °C, which is slightly lower than the peak metamorphism of this region, and the modal abundance of garnet is the highest along the metapelite–metabasite boundary (up to 40%), which is consistent with the field and thin section observations. The occurrence of brine (7.0–10.9 wt.% NaCl_eq for ice melting or 25.1–25.5 wt.% NaCl_eq for hydrohalite melting) fluid inclusions as a primary phase trapped within plagioclase in the garnet-rich layer and the occurrence of Cl-rich biotite (Cl = 0.22–0.60 wt.%) in the metasomatic rock compared to that in pelitic (0.15–0.24 wt.%) and mafic (0.06–0.13 wt.%) granulites suggest infiltration of brine fluid could have given rise to the high-temperature metasomatism. The fluid might have been derived from external sources possibly related to the formation of major suture zones formed during the Gondwana amalgamation.