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Cambridge Coins in Signet Court was hit by thieves on Thursday 20 February.
Two men targeted the shop just off Newmarket Road using a ladder and a brick at just after 3am, and it is believed about £40,000 worth of rare coins were taken. The men had left the area when police arrived.
At 10pm on the same day, the coin dealer was targeted for the second time. Four masked men forced entry using a disc cutter, sledgehammer and crowbars.
The men, who wore gloves and balaclavas, found a safe inside that contained about £10,000 worth of silver coins. The entire safe was thrown from the first-floor window and taken by the suspects, who fled the scene in a blue Audi.
Officers searched the surrounding area but to no avail.
An investigation has been launched into both crimes, and officers are appealing for witnesses. It is not known if the two break ins are linked, but police are keeping an open mind.
Detective Sergeant Jon Lockwood from Cambridgeshire Police:
“We are urging anyone who saw anything suspicious in the area at any point yesterday, be that in the early hours or later the same day, to get in touch with us.
“This includes any CCTV or doorbell footage, anyone with dashcam footage of a blue Audi in the area, or anyone who saw people acting suspiciously nearby.
“No matter how small or insignificant the information may seem, it could help more than you think. Information can also be submitted anonymously via Crimestoppers.”
Anyone with any information is urged to report this to police online or by calling 101, quoting crime reference numbers 35/12349/25 and 35/12599/25.
Alternatively information can be submitted anonymously via Crimestoppers by calling 0800 555111 or online at www.crimestoppers-uk.org.