Lammtarra, the unbeaten winner of the Derby, King George and Prix de l'Arc de Triomphe in 1995, has died at the age of 22.
Godolphin's Saeed bin Suroor led the tributes to Lammtarra, describing him as one of the best he has ever trained.
Originally trained by the late Alex Scott as a two-year-old, he won the blue riband at Epsom in the care of Bin Suroor after Scott was murdered in September 1994, a month after the son of Nijinsky had won the Washington Singer at Newbury.
He raced in the name of Sheikh Mohammed's nephew Saeed Maktoum Al Maktoum as a juvenile before being part of Godolphin in his Classic season, during which he added the two all-aged middle-distance championships of Europe to his Epsom laurels.
"It is very sad. He is one of the best horses I have trained," Bin Suroor said.
"He won the Epsom Derby, the King George and the Arc. Very few horses have managed to win those three races.
"He was a great horse, it is sad to lose him and we will miss him, but he will be remembered forever."
Darley said the chestnut was euthanised at Dalham Hall Stud following a short illness.
Lammtarra was ridden by Walter Swinburn at Epsom, then Frankie Dettori took over at Longchamp for the Arc.