Captain Paul McGinley announced that the vastly experienced trio - who have played in 17 Ryder Cups between them - will join Des Smyth and Sam Torrance as his deputies at Gleneagles later this month.
Olazabal led Europe to their famous comeback victory at Medinah in 2012, while his fellow Spaniard Jimenez served as one of his vice-captains two years ago. Jimenez was also Seve Ballesteros' right-hand man in 1997.
And while Harrington has never been a vice-captain before, the three-time major winner has played in six Ryder Cups between 1999 and 2010 – winning on four occasions.
Wednesday's announcement means McGinley will have five vice-captains to lean on at Gleneagles, and the Irishman expressed his delight at the support network he has assembled.
"They will all bring valuable insight and experience to the players and the team room," explained McGinley.
"Padraig is my oldest friend on Tour and is a guy I have known most of my life…so I know what he can bring to the team room.
"As far as Miguel is concerned, he is someone that the spectators love as well as being very popular with all the players [and] he is also a person that I respect very much.
"Finally, Jose Maria's passion for the Ryder Cup is recognised the world over - it was obvious in his legendary partnership with Seve and was also so very apparent two years ago at Medinah."
Europe's quest to retain the Ryder Cup begins on September 26.