According to Scotland Yard, the robbers, smashed glass cabinets at the Selfridges department store to steal high value watches.
The group of men fled the shop and are reported to have made their getaway on mopeds and motorbikes, ridden by associates.
Two suspects were later arrested when they came off a moped and members of the public stopped them fleeing.
Detectives from the Metropolitan Police's Flying Squad are investigating the incident.
More From This Section
"I'd like to thank those members of the public who stepped in and detained our two suspects. Their quick thinking and brave actions have helped our investigation," he added.
Police have recovered a number of watches from near the scene of the crash.
One of the men was arrested in connection with the robbery and taken to a central London police station where he remains in custody.
Two other motorbikes, believed to have been used in the gang's getaway, have been recovered by police in the Paddington area.
A message posted on Selfridges' Twitter feed read: "Hi, we just want to let you know that everyone is safe and the police are investigating. We will update you once we have more information."
The raid took place 30 minutes before the world famous department store was due to close at 2100 local time yesterday.
Onlookers posted photographs of the scene on Twitter, including one showing tiny pieces of broken glass and another showing two axes.
The flagship store in London's Oxford Street is the second largest shop in the UK after the equally famous Harrods.