Gold Rosary Beads carried by Mary Queen of Scots at her execution in 1587 are among the items stolen.
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British police are appealing for information after historical items worth over £1 million (€1.15 million) were stolen from Arundel Castle.
The break-in at Arundel Castle, in Sussex, south-east England, took place on Friday evening.
"Various items have been stolen of great historical significance," Sussex police said on Sunday.
These include the Gold Rosary Beads carried by Mary Queen of Scots at her execution in 1587, several coronation cups and other gold and silver treasures.
They were all taken from a display cabinet along the public route.
"The stolen items have significant monetary value, but as unique artefacts of the Duke of Norfolk's collection have immeasurably greater and priceless historical importance," a spokesman for Arundel castle Trustees said.
Police are now examining a 4x4 vehicle found abandoned and on fire in nearby Barlavington to establish whether it is connected to the burglary and are appealing for information.
The monument only reopened to the public on May 18.