We present a new geological map and new structural, petrographical and geochronological data from the Uppermost Unit of the Cretan nappe pile exposed south of the Dikti Mountains in eastern Crete (Greece). Based on these data, the Uppermost Unit in the study area can be subdivided (from bottom to top) into the Arvi Unit, Theodorii Greenschist and Asterousia Crystalline Complex (ACC)-type rocks. The ACC-type rocks have been affected by polyphase deformation (D1–D3) and metamorphism. Relics of the D1 phase are preserved as internal foliation in garnet porphyroblasts. D2 top-to-the SE shearing under upper amphibolite facies conditions led to the dominant foliation. After post-D2 exhumation, parts of the ACC-type rocks were affected by contact metamorphism of a non-exposed pluton, which intruded at a depth below 10 km during Campanian time (74±2 Ma; laser ablation inductively coupled plasma mass spectrometry on zircon). This age, obtained from zircon of chiastolite hornfels, is in line with intrusion ages of ACC-type (meta)granitoids exposed on Crete and on Anafi. The S2-foliation of the ACC-type rocks was reactivated during the late phase of contact metamorphism by D3 top-to-the SE shearing. Latest Cretaceous cross-mica with low silicon content post-dates this shearing event. During middle Paleocene time, the ACC was thrust on top of the Theodorii Greenschist. This thrusting event as well as subsequent brittle thrusting of the greenschists and the ACC-type rocks on top of the prehnite-pumpellyite facies metamorphic Arvi Unit was still accommodated by top-to-the SE kinematics, which is the dominant kinematics of the Uppermost Unit on Crete and on Anafi.