Various earthquake source models predict that aseismic slip modulates the seismic rupture process. However, observations of aseismic slip associated with earthquakes are scarce, which has left the earthquake source model controversial. Here, we characterise seismic and aseismic processes for 3 days during the 2014 Iquique earthquake sequence in northern Chile by analysing seismicity and crustal deformation time series measured by high-rate Global Positioning System (GPS). We demonstrate that the early afterslip started immediately after the M 8.1 mainshock and led to the largest M 7.6 aftershock 27 hours later, located ~120 km to the south. At the mainshock latitude, the interevent early afterslip is located downdip of the mainshock rupture, and is associated with aftershocks. These afterslip and aftershocks exhibit a rapid temporal decay. In contrast, south of the mainshock slip patch, a peak of afterslip separates the mainshock rupture from the largest aftershock, suggesting that this area acted as a barrier to the southward propagation of the mainshock rupture. Seismicity count and moment accelerate in this southern area during the interevent stage. We conclude that the largest aftershock nucleation was driven by the interevent afterslip. The mechanical connection between sequential great earthquakes can therefore be mediated by aseismic slip.