The Payer Land gneiss complex is unique among the mostly amphibolite-facies, mid-crustal gneiss complexes in the East Greenland Caledonides due to its well-preserved, regional high-pressure (HP) granulite-facies metamorphism. High-pressure – high-temperature (HP–HT) assemblages are recognized in mafic, ultramafic, granitic, and metasedimentary lithologies. Anatectic metapelites contain the assemblage garnet + kyanite + K-feldspar + antiperthite (exsolved ternary feldspar) + quartz ± biotite ± rutile and record approximately the same peak metamorphic conditions (pressure (P) = 1.4–1.5 GPa, temperature (T) = 800–850°C) as those of the neighboring mafic HP granulites. The HP granulite-facies metamorphism is Caledonian based on in situ U–Th–Pb electron microprobe dating of monazite from two samples of the aluminous paragneiss. The monazites are found along garnet–kyanite phase boundaries, as inclusions in garnet and kyanite, and within small leucocratic melt pods (K-feldspar + plagioclase + kyanite ± garnet) within the HP–HT paragneisses. Mylonitic equivalents of the metapelites contain a detrital monazite age signature that suggests the Payer Land paragneisses correlate with other Mesoproterozoic metasedimentary sequences in the area. The gneisses form a metamorphic core complex that is separated from the overlying low-grade sedimentary rocks of the Neoproterozoic Eleonore Bay Supergroup by an extensional detachment. This newly recognized Payer Land detachment is part of a system of prominent extensional faults located in the southern half of the Greenland Caledonides (i.e., south of 76°N). The HP granulites preserve the deepest level of crust exposed in this southern segment of the orogen and attest to significant crustal thickening.