The Santiago Peak volcanics, in the northern Santa Ana Mountains, are the northernmost exposures of the Santiago Peak–Alisitos magmatic arc present along the western edge of the Peninsular Ranges batholith. Remnants of deeply eroded volcanic sequences in the Santa Ana Mountains consist of subaerial basaltic-andesite to rhyolite lavas, rare basalt, welded tuff, and pyroclastic rocks that were emplaced across deformed Middle Jurassic turbidites. Subalkaline lavas have mixed calc-alkaline and tholeiitic affinities. Relatively primitive ε_Sr (−18 to +5) and ε_Nd (+7.5 to +0.1) values for the lavas plot along the mantle array. Silicic lavas have higher ε_Sr and ε_Nd values in comparison to mafic lavas. Parental magmas were derived from hydrous melts of relatively depleted mantle wedge, followed by fractionation and the assimilation of up to 10% crustal materials. The whole-rock compositions, isotopic data, and U/Pb and ⁴⁰Ar/³⁹Ar ages (128–110 Ma) of the Early Cretaceous Santiago Peak volcanics and related Estelle Mountain volcanics overlap with emplacement ages of plutons of the western zone of the Peninsular Ranges batholith. The volcanic rocks are interpreted as the volcanic component of the arc plumbing system of the batholith. Arc rocks are in turn unconformably overlain by a forearc sequence of Upper Cretaceous through Tertiary strata that indicate deep erosion of the Santiago Peak volcanics by 95 Ma. Volcanic clasts of Turonian age within the forearc sequence yield U/Pb ages of 108–106 Ma. Age data and whole-rock geochemistry of the volcanic clasts indicate that they were eroded from supracrustal volcanic rocks located farther east within the Elsinore block.