Without a doubt, the most significant artefact of the monastery is the piece of the Holy Cross which bears an impression of the nails from the Crucifixion of Christ. It is one of the largest surviving pieces of the Holy Cross, and was donated by the Emperor Romanos I Lekapinos to the founder of the Monastery, St Pavlos. In addition, the Monastery has ten magnificently-crafted chests which contain segments of the Holy Gifts (gold, frankincense and myrrh) brought by the Magi to the infant Christ. The Holy Gifts were donated to the Monastery by the venerable Queen Maro, the daughter of the Serbian ruler Branković (1428-1456), who greatly helped the Monastery.
Among the treasures of the Monastery are the large number of miraculous and myrrh-emitting sacred relics belonging to more than 100 saints of the Orthodox church. The relics are kept in exquisitely-crafted reliquaries in the holy altar of the cathedral and are exhibited for veneration by the public during the celebration of the respective feast day of each saint.