As an important part of the early Mesozoic granites in the South Qinling tectonic belt (SQTB), the Guangtoushan pluton provides a material basis for research on the composition of magma sources and the effects of peritectic assemblage entrainment (PAE) on the changes in the granite composition. As shown by the results of LA-ICP-MS zircon U-Pb dating, the Guangtoushan pluton was emplaced during the Late Triassic (214–212 Ma) and was formed in the post-collision stage between the SQTB and the Yangtze plate. The collected samples had high SiO2 content and low Cr and Ni contents, indicating that the magmas did not undergo significant crust-mantle mixing during their evolution. The Guangtoushan granitoids were distributed along the trend line of magmatic fractional crystallization in the F–An–Or diagram. This result, combined with the relatively homogeneous Sr-Nd isotopic composition, implies that the Guangtoushan pluton underwent slight assimilation and contamination. As can be inferred from the comparison between the compositions of the Guangtoushan granitoids and various fluid-absent experimental melts, the magma sources of the Guangtoushan granitoids contain a variety of materials, such as graywackes, pyroclastic graywackes, and pelites and are not derived from lower crustal mafic rocks. The correlation between the maficity and the major and trace elements further indicates that the strongly peraluminous granitoids from the Guangtoushan pluton was formed by the partial melting of biotite-bearing crustal rocks and its magmatic evolution was accompanied by the entrainment of clinopyroxenes and accessory minerals.