The Metropolitan Police said that it received reports of an aggravated burglary at the store at 12:45am on Monday.
Thousands of pounds worth of iPhones, iPads and watches were stolen after the gang broke into the building, and a security guard was threatened with a hammer when he attempted to confront the thieves.
Mounted on five mopeds, the gang were inside the store for less than three minutes, with look-outs reportedly posted outside the store while others snatched items on display stands.
Two iPhone Xs were later recovered near King's Cross.
A red scooter was left abandoned inside the glass doors of the store and detectives are combing through CCTV recordings of the robbery.
It is the latest raid and one of the most high-profile of an increasingly visible burglary tactic in recent weeks.
Last month, thieves riding mopeds burgled the high-end Mappin & Webb jeweller's store in the same street.
Official figures suggest that there are on average 53 moped-enabled crimes in London every day, including thefts and robberies.(c) Sky News 2017: Apple store raided by hammer-wielding moped gang