The terror suspect was caught by a plain-clothes officer on Saturday, four days after escaping from prison.
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Terror suspect Daniel Khalife remains in police custody after being arrested in north-west London on Saturday.
The 21-year-old was apprehended by a plain-clothes officer who pulled him from a bicycle on a canal towpath in the Northolt area.
The arrest followed a four-day search after Mr Khalife’s escape from Wandsworth prison.
The Met said he had been arrested on suspicion of being unlawfully at large and being an escaped prisoner.
The former soldier was detained at 10:41 BST on Saturday, about 14 miles from the prison he escaped on Wednesday morning.
Police had offered a reward of up to £20,000 for information leading to his arrest and detectives said they had received more than 100 calls from people offering information. The reward has not been claimed yet.
Video footage obtained by The Sun newspaper showed him sitting on the canal towpath after his arrest, with a bike, a Waitrose cool bag and a sleeping bag nearby.
Cdr Dominic Murphy, head of Counter Terrorism Command, told reporters Mr Khalife was “fully co-operative” as he was handcuffed.
Elsewhere, the Mail on Sunday reports claims from security sources that Mr Khalife was apprehended after spies from the UK’s new intelligence nerve centre, made up of agents from MI5, MI6, and specialist police, bugged the phones of people they believed were linked to him.
How police closed in on Daniel Khalife
The Met said earlier on Saturday morning it was focusing on “intensive search activity” efforts in and around the Chiswick area of west London, where Mr Khalife had been spotted by members of the public.
One woman, who lives in Chiswick, told BBC News she believed she briefly spoke to him as he sat on a bench in Chiswick House Gardens on Friday morning.
After commenting on the hot weather, she said he claimed he had just come out of the Army. She described him as gentle and sweet, and said he was affectionate towards her dog.
Police originally said Mr Khalife was held in the Chiswick area but later clarified he had been detained several miles away in Northolt.
Cdr Murphy said the investigation “took a different course” on Friday night, when officers conducted an “intelligence-led search at a residential premises” in the Richmond area.
While Mr Khalife was not found there, the force received a number of calls from the public with sightings of the suspect nearby.
Police said on Friday that Mr Khalife had been spotted emerging from underneath a lorry at Wandsworth Roundabout shortly after he escaped.
His escape began in the kitchens of the prison – where he held a job – after he attached himself to the underside of a food delivery lorry.
Police hunt for Daniel Khalife
Mr Khalife is accused of trying to spy for an enemy state, understood to be Iran, obtaining information likely to be useful to a person committing or preparing an act of terrorism, and plotting a fake bomb hoax.
He was at Wandsworth on remand pending a trial in November after being denied bail at a court hearing in January.
Justice Secretary Alex Chalk said he would leave “no stone unturned” in the investigations into prison security and categorisation.
Writing on social media, shadow home secretary Yvette Cooper said “we need answers about how on earth a prisoner charged with terror and national security offences could have escaped in this way”.