Archean granitoids played key roles in the generation and differentiation of the Archean continental crust and provide clues to understand crustal processes in the early Earth. Abundant Mesoarchean granitoids were emplaced in the Nyabessane granite-greenstone terrane (NGB), part of the Ntem Complex of the Northwest Congo Craton. They include charnockites, tonalite-trondhjemite-granodiorite (TTG), granitic and monzogranitic gneisses. Here, we present a geochemical and geochronological (zircon LA-ICP-SF-MS UPb) study of these granitoids to determine their petrogenesis and to better constrain the crustal evolution of the Ntem Complex. Field and petrographic observations indicate that most of these granitoids underwent extensive metamorphism and deformations, associated with anatexis. Zircon UPb dating results suggest that the charnockite, TTGs and granitic gneisses, and monzogranites have emplacement ages of 2910 ± 11 Ma, 2870–2865 Ma and 2852 ± 31 Ma, respectively. The charnockites have low SiO2 (55–58 wt%) and high Al2O3 (16–18 wt%), CaO (7–8 wt%) and MgO (∼ 4.5 wt%) content with Mg# ∼ 54, and exhibit magnesian, metaluminous characteristics of the Cordilleran granitoid-type formed in magmatic arc. The 2.87–2.86 Ga TTG gneisses are silica-rich (55–58 wt% SiO2), sodic (3–5 wt% Na2O, Na2O/K2O = 1–3), with HREE-depleted, and display the typical Archean medium- to low pressure TTG geochemical features groups. Their chemical compositions are characteristics of TTG-like melts derived from the partial melting of hydrated low- to high-K metabasic/thickened lower crust at various depths followed by magmatic differentiation during ascent. When compared to the TTG gneisses in the NGB, the ∼2.87 Ga granitic gneisses are K-rich, and high Gd/Yb, Th/Yb, Th/Nb, Sr/Y and La/Yb ratios but lower MgO, Yb, V, Y, Cr, Ni and Sr contents, matching typical Archean hybrid and potassic granitic rocks. We propose that the granitic gneisses were derived from the intra-crustal melting of a pre-existing felsic crust. The granitic and the TTG gneisses were generated contemporaneously through the same magmatic event at ∼2.87–2.86 Ga. The ∼2852 Ma monzogranitic gneisses are ferroan and metaluminous rocks, and show LREE enrichment with strongly fractionated REE patterns and positive Eu anomalies. Geochemical features, together with the presence of ∼2.9 Ga-old inherited zircon grains are consistent with the remelting of Mesoarchean granitoids. Considering the petrogenetic, regional geological and geochronological data, the Mesoarchean granitoid magmatism of the Ntem Complex was likely generated via complex transitional geodynamic regimes involving subduction and accretion processes.