AbstractVarious earthquake models predict that aseismic slip modulates the seismic rupture process but actual observations of such seismic‐aseismic interaction are scarce. We analyze seismic and aseismic processes during the 2014 Iquique earthquake sequence. High‐rate Global Positioning System displacements demonstrate that most of the early afterslip is located downdip of the M 8.1 mainshock and is accompanied by decaying aftershock activity. An intriguing secondary afterslip peak is located ∼120 km south of the mainshock epicenter. The area of this secondary afterslip peak likely acted as a barrier to the propagating mainshock rupture and delayed the M 7.6 largest aftershock, which occurred 27 hr later. Interevent seismicity in this secondary afterslip area ended with a M 6.1 near the largest aftershock epicenter, kicking the largest aftershock rupture in the same area. Hence, the interevent afterslip likely promoted the largest aftershock nucleation by destabilizing its source area, favoring a rate‐dependent cascade‐up model.