The retired detective chief superintendent was known as "Slipper of the Yard."
He came to public attention for his role in the "Great Train Robbery" of 1963, one of Britain's largest and most audacious heists and a crime that still fascinates the country.
An armed gang held up the Glasgow-to-London mail train, stealing 125 sacks of banknotes worth 2.6 million pounds — valued at $7.3 million at the time, or more than $50 million today.
The train's driver, Jack Mills, was hit over the head during the robbery. Mills never returned to work and died of cancer in 1970.
A team of detectives, including Slipper, arrested most of the gang soon after the robbery. But one member, Ronnie Biggs, escaped from prison after 15 months by scaling a wall with a rope ladder and jumping into a waiting furniture van. Biggs fled to Spain, had plastic surgery to change his appearance, spent several years in Australia, and settled in Brazil in 1970.
In 1974, Slipper traveled to Rio de Janeiro to arrest Biggs. Brazilian authorities refused to hand him over, because Biggs' Brazilian girlfriend was pregnant. As the father of a Brazilian dependent, he could not be deported.
Biggs eventually returned to Britain in 2001, in failing health after a series of strokes, and was jailed in Belmarsh Prison.
Slipper acknowledged a grudging respect for his adversary. In 1994, he called the train robber "a villain and a cunning monkey," but added: "When it comes to the important things in life, like his son and family, he seems to be an honest man."
Biggs' son, Michael, said the family is saddened by Slipper's death.
"Even though my father and Mr. Slipper were on different sides of the fence, there was a very high and mutual respect between them," Biggs said.
The Metropolitan Police said that despite his high-profile association with the train robbery, Slipper had gained the most satisfaction from bringing to justice the killers of three London policemen in 1966.
Former detective Mike McAdam, a friend, called Slipper "one of the finest detectives in the last century."
"New Scotland Yard has a worldwide reputation and the name Jack Slipper, or 'Slipper of the Yard,' is synonymous with the Yard," McAdam said.
Slipper is survived by his wife, Annie, two daughters and five grandchildren.
By Jill Lawless