The gems that adorn two golden chalices from Einsiedeln Abbey (Switzerland) crafted in 1609 and 1629 were investigated using Raman spectroscopy. The results were also compared with those obtained by other non-destructive means such as microscopy and energy-dispersive X-ray fluorescence. The chalice made in 1609 was adorned with 16 corundum (15 rubies and 1 sapphire), four garnets (two almandine and two grossular), seven quartzes (six amethysts and one citrine) and one peridot (forsterite olivine). All pearls of this chalice were found to be from a saltwater mollusc. The chalice crafted in 1629 was adorned with 23 diamonds. Compilation of all the results does not exclude that the stones mounted to the chalices are of ‘oriental’ origin. However, more research needs to be done by additional spectroscopic means to shed more light on their origin. Copyright © 2012 John Wiley & Sons, Ltd.