New, detailed geological/structural mapping and field-based structural analysis were carried out to investigate the deformation pattern of well-preserved high-pressure rocks of the Blueschist Unit exposed in SE Syros (Cyclades, Greece). Geological mapping revealed the occurrence of extensive alternations between different rock groups, as well as interfingering patterns in map-scale that are possibly the result of folding. The earlier ductile deformation phase recognized in the mapped area is associated with the development of a penetrative foliation, which was formed at eclogite/blueschist-facies conditions under peak metamorphism. The subsequent main deformation phase occurred under blueschist facies conditions synchronous with the early stages of exhumation of the high-pressure rocks. This phase is mainly associated with the formation of WNW-trending folds and a pervasive axial planar foliation linked with ESE-directed shearing. The main deformation ceased under blueschist-facies conditions, and exhumation of the rocks to greenschist-facies conditions took place under very weak and localized deformation. Greenschist retrogression observed in the southwestern part of the mapped area seems to be controlled by fluids, rather than by intense deformation and formation of major syn-greenschist shear zones.