In the Bonfim W–Mo and Au–Bi–Te skarn deposit, Northeastern Brazil, Archean metamafic–ultramafic rocks are similar to those found in greenstone belt sequences worldwide. The Bonfim emerald deposit comprises metric layers of lenticular-shaped phlogopite-rich schist developed at the symmetrical contacts between metamafic–ultramafic rocks and Be-rich granite intrusions. They formed near these rocks by metasomatic fluids emanating from granitic magma. Metasomatism also transformed the marble and schists into skarns at the marble–schist contact and within the marble. This contribution describes the drill cores containing Mg-rich schist in the Neoproterozoic metapelitic sequence. Detailed petrographic observations and geochemical analysis reveal that it contains phlogopite, anthophyllite, fuchsite, and anomalous Cr–Ni–V–Co–Sc contents. These characteristics contrast those of the common schists at Bonfim or regionally and indicate a probable komatiitic affinity. The anthophyllite–phlogopite-bearing schist contains a metamorphic paragenesis of phlogopite + anthophyllite + garnet + tourmaline + zircon + monazite + plagioclase + quartz, followed by two successive retrograde metasomatic parageneses comprising (i) clinozoisite–zoisite + apatite and (ii) white mica (±fuchsite) + clinochlore + quartz. It exhibits a peculiar texture containing prismatic pseudomorphs (1–7 mm long) composed of anthophyllite, clinozoisite–zoisite, and white mica. The relict orthogonal cleavage suggests that they could represent preexistent Mg-rich pyroxene. Similar to the common schist in Bonfim, the anthophyllite–phlogopite-bearing schist near the skarns is metasomatically converted in places into actinolite–anthophyllite–phlogopite-bearing schist. The anthophyllite–phlogopite-bearing schist contains phlogopite and biotite with low Fe/(Fe + Mg) (between 0.2 and 0.4) and anthophyllite with a composition close to Mg5Fe2Si8O22(OH)2 (MgO approximately 22 wt% and Al2O3 <0.7 wt%). In the actinolite–anthophyllite–phlogopite-bearing schist, the metasomatically formed amphibole has a composition varying from actinolite to magnesiohornblende with a high MgO (>16.5 wt%). The whole-rock geochemical analyses of three representative samples indicate that the anthophyllite–phlogopite-bearing schist contains high MgO (approximately 15%), Cr (up to 574 ppm), and Ni (up to 237 ppm) contents, besides V (up to 198 ppm), Co (up to 51 ppm), and Sc (up to 25 ppm). The anthophyllite–phlogopite-bearing schist has higher MgO, K2O, S, Cr, Co, Ni, and Rb contents, and lower Na2O, P2O5, Zn, Sr, Zr, and Pb contents than the average composition of the Seridó regional schist. The 87Sr/86Sr ratio in two representative samples of the Bonfim schists revealed that the anthophyllite–phlogopite-bearing schist has higher ratio (0.89455) than the enclosing common schist (0.74514), indicating distinct ages of the source rocks for the sedimentary protolith of these two schists, with evidence for an older age of the former source. The original sediments of the anthophyllite–phlogopite-bearing schist could have had an Archean komatiitic source (e.g., komatiitic basalt, peridotite, websterite or pyroxenite), as indicated by the Mg-rich metamorphic minerals (phlogopite and anthophyllite), Cr–K-rich metasomatic ones (fuchsite), and the peculiar MgO, Cr, Ni, Co, Sc, and K2O contents. This source could be part of an Archean greenstone belt now dismantled and/or removed by tectonic and erosion processes. Alternatively, the Mg-rich schist could be a remnant of the upper sedimentary unit of such an ancient rock sequence. The unusual schist could potentially guide gold and emerald deposit prospecting in the region.