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Officers have now sealed off the corner of Dorset Square and Balcombe Street, in Marylebone, after a car chase through the West End during which shots were fired.
The gunmen are believed to be members of an IRA hit squad which has been behind a number of attacks in the capital and home counties over the past few months.
They are accused of shooting dead TV presenter Ross McWhirter at his Enfield home a week ago, and also of carrying out attacks on London restaurants, the Hilton hotel and the Army public house at Caterham in Surrey.
Lying in wait
The couple being held hostage are John Matthews and his wife Sheila. There are reports they have a young child as well, although these have not been confirmed.
Police appear prepared for a long siege. A large mobile headquarters has been brought in and there is an army personnel carrier in a nearby street where several diplomats are believed to live.
Donna Martin, who lives in Dorset Square overlooking the siege address, was watching from her window:
"About 50 cars arrived at my doorstep. We all rushed to the window and I have never seen so many guns in my life. We saw the policemen with a car which was riddled with bullets.
"Then the police came into our flat. They all had guns and were wearing flak jackets."
The gunmen were cornered after they attacked Scotts restaurant, in Mayfair.
It was the second time the building had been targeted. On 12 November a bomb containing ball-bearings was thrown into the restaurant, killing one and injuring 15 others.
This time, police were lying in wait and when the gunmen opened fire from their car, a Cortina, they were ready to give chase.
The Cortina was pursued through the busy West End traffic to Gloucester Place in Marylebone. A number of shots were fired and the windscreen of the getaway car was shattered.
The driver could no longer see where he was going and stopped the car. Police later found a holdall in the car containing two sub-machine guns, a Sten gun barrel and a clip of ammunition.
The four gunmen ran down Balcombe Street and finally burst into a five-storey block of flats owned by Westminster City Council.
Mrs Matthews is reported to have opened the door of flat number 22B to see what all the noise was about and the men smashed their way past her and barred the door.
The Balcombe Street siege lasted six days.
The gang demanded safe passage to Ireland, but the police, led by chief negotiator Detective Superintendent Peter Imbert (later Metropolitan Police Commissioner 1987-93) was adamant there would be no deals.
On the second day of the siege, police were able to speak to Mrs Matthews using a phone which had been passed down through the window from the flat above. There was no child in the flat.
The gang and their hostages were held in a single room, with no access to running water or a toilet. Although police initially refused requests for food, they did give them water and a chemical toilet.
The gunmen later broke off negotiations by throwing the phone out of the flat window and police had to resume talks with a loud hailer. The first sign of weakness was when the terrorists asked to restore the phone link.
The four gunmen eventually surrendered themselves to detectives.
The "Balcombe Street Gang" - Martin O'Connell, Edward Butler, Harry Duggan and Hugh Doherty, were jailed for life but later freed under the terms of the Good Friday agreement.
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