Austin Caballero, 42, went uncaught for more than two-and-a-half years, in one case being recorded on camera grabbing a £9,500 bronze statue and sliding it into his jacket.
The Met's Super Recogniser Unit - a squad of specialist CCTV analysts - pored over dozens of clips of him pilfering jewellery, designer clothing, handbags, high-end cosmetics, sunglasses and even antiques from shops in the capital's most upmarket areas.
The brazen shoplifter, who police believe was "under the illusion that he would never be captured", has now finally been caught, The Press Association reported.
The unit spotted the thief, often smartly dressed, boldly committing crimes in shops across London.
On Friday, Caballero, of no fixed address, finally admitted 40 counts of theft at Blackfriars Crown Court, where he was jailed for nearly four years.
Between April 30 2013 and December 22 2015 he swiped expensive goods from shops in Westminster, Kensington and Chelsea and Camden.
CCTV released by police revealed the extraordinary extent to which the audacious opportunist would go to make a dishonest living.
Caballero hit one boutique posing as a respectable customer, only to slip a £580 bottle of beauty cream into his jacket when staff turned their backs.
In another clip Caballero could be seen stuffing three cashmere scarves worth £1,200 into his trousers before resuming his act of an innocent browser.
Then on a separate occasion he waited for a jeweller to turn her back before swiftly pocketing two bracelets worth £8,500.
After appearing on camera several times he was eventually identified by one of the Met's eagle-eyed super recognisers - officers with a sharpened ability to recognise individuals in CCTV footage.
In August detectives launched a public appeal to find the thief and he was arrested on New Year's Day.
Detective Sergeant Eliot Porritt, of the Super Recogniser Unit, said: "Caballero has been brazen during his relentless spree of offences.
"Given the time period and frequency of offences, I have no doubt that he was under the illusion that he would never be captured.
"My unit scans thousands of images in order to link offenders to their crimes, resulting in a greatly reduced cost to the public of just one court process as opposed to the dozens of separate cases that could have resulted had he not been recognised and linked by my team."
By the time he was arrested the eagle-eyed officers had linked Caballero to 41 offences with CCTV footage and evidence.
They included 40 thefts and one count of racially aggravated assault.
He was sentenced to three-and-a-half years for the theft offences and an additional three months for the assault.
After failing to attend court over the thefts he was sentenced to a further nine months in prison, although a judge ruled it could be served concurrently.