New 40 Ar/ 39 Ar results from drill-hole cuttings of basaltic and basaltic andesite flows from the Guaje well field of the Pajarito Plateau along the western part of the Española Basin in north-central New Mexico yielded Middle Miocene ages (11.5–13.2 Ma). The volcanic eruptions were closely associated with intense faulting, subsidence, and sedimentation, and the results provide age constraints for the volcanic and tectonic processes along the western margin of the Española Basin. The Middle Miocene volcanic rocks are interbedded within the Santa Fe Group, which is divided into the Hernandez and Vallito Members of the Chamita Formation and the Chama–El Rito Member of the Tesuque Formation, in descending stratigraphic order. New and published geochemical results from the Guaje well field and from other surface and subsurface mafic and intermediate lava flows within the Pajarito Plateau suggest that the volcanic rocks erupted from different magmatic sources and centers close to the Pajarito fault zone. Multiple pulses of volcanic eruptions mostly confined to the hanging wall of the Pajarito fault zone, which represents the current western boundary fault of the Española Basin, suggest that the Pajarito fault system has been sporadically reactivated several times, beginning at least in the Middle Miocene and continuing to the Plio-Pleistocene. Moreover, the volcanic, tectonic, and sedimentary records in the Pajarito Plateau suggest that there is no evidence for eastward migration of tectonic and volcanic activities from the Cañada de Cochiti fault zone in the southern part of the Jemez Mountains to the Pajarito fault zone during the early Pliocene (4–5 Ma).