Grosvalet said the theft was particularly disturbing as the reliquary had been saved from being melted down during the turmoil following the French Revolution in 1789.
The reliquary, topped by a gold crown with nine 'fleurs-de-lis', the lily-shaped royal motif, is considered a masterpiece. It was displayed at the museum for more than 130 years.
Catherine Touchefeu, a departmental councillor, urged the robbers to return it. "If the thieves were motivated by the fact that it is shiny and made of gold, they should understand that its historical and symbolic value far outweighs its 100 grams of gold."
After Anne's death in 1514, she was buried, as custom dictated, alongside other French royals in the Basilica of Saint Denis outside Paris. But to show that her heart belonged to Brittany, it was placed in her parents' tomb at the chapel of the Carmelite friars in Nantes, in accordance with her wishes. As queen she defended the autonomy of Brittany, then a duchy linked by treaty to France and often referred to as "Little Britain".
Reputed to be the richest woman in Europe, her hand was eagerly sought by many kings. In 1483, her father arranged for her to marry the Prince of Wales, Edward, but the young prince disappeared, presumed to have been killed by his uncle Richard III.
She married Charles VIII of France in 1491, ascending the throne as queen consort at the age of 12. As he died without an heir in 1498, she married Louis XII a year later and became the only woman to be crowned queen of France twice.
Louis, grief-stricken when she died in 1514 at the age of 36, is said to have wept for eight days and ordered her tomb to made large enough for two.