The 595–560 Ma post-collisional magmatism in the Alto Pajeú Domain, Borborema Province, northeastern Brazil, is characterized by the intrusion of voluminous high-K calc-alkaline, shoshonitic and ultrapotassic magmas. The nature of the source rocks and the geodynamic context associated with the generation and emplacement of this post-collisional magmatism is still enigmatic. In this study, we report new UPb ages, elemental geochemistry, mineral chemistry and SrNd isotope data for rocks from the Pajeú batholith. LA-ICP-MS zircon UPb dating revealed that this batholith was formed by at least two distinct magma pulses. The oldest pulse (ca. 592 Ma) consists mainly of porphyritic quartz monzonites to monzogranites with abundant mafic microgranular enclaves (MMEs), while the younger pulse (ca. 568 Ma) is composed of equigranular biotite granites. The porphyritic monzogranites are magnesian, have intermediate to acidic compositions (SiO2 = 62.2–67.6 wt%) and high Mg# (44–55) values. In contrast, biotite granites are ferroan, have high SiO2 (69.3–73.1 wt%) and low Mg# (16–36) values. Both rock types are characterized by enrichment in LREE and LILE and depletion in HREE and HFSE, but with more fractionated REE patterns for biotite granites ([La/Yb]N = 67.4–101.5) than for porphyritic rocks ([La/Yb]N = 35.8–54.8). The SrNd isotopic values for the different rock types are roughly similar. However, biotite granites show slightly higher initial 87Sr/86Sr (0.71265–0.71412) ratios and more negative εNd (t) (−18.45 to −18.67) values than porphyritic monzogranites (initial 87Sr/86Sr ratios from 0.71077 to 0.71155 and εNd (t) from −16.04 to −16.96). These geochemical and isotopic signatures, together with mineral chemistry data, suggest different sources for the two rock types. The biotite granites are of purely crustal origin, derived by partial melting of a Paleoproterozoic amphibolitic lower continental crust, while a mixture of melts derived from the Paleoproterozoic continental crust and magmas derived from an enriched lithospheric mantle could explain the origin of porphyritic monzogranites. Based on the spatial and temporal distribution of magmatic rocks from the Alto Pajeú Domain, we suggest that a local lithospheric thinning model could explain the evolution of post-collisional magmatism in this region of the Borborema Province.