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Sunday’s final round promises to be a definitive occasion for McIlroy one way or the other, as he chases a fifth Major title having last claimed such a triumph eight years ago.
Only a bogey on the famous Road Hole 17th prevented McIlroy from holding the outright lead, with Ryder Cup teammate and playing partner Hovland, chasing his first major title, carding a bogey-free 66 to join the Northern Irishman on 16-under.
McIlroy lifted the Claret Jug in 2014 and won his fourth major in the US PGA a month later, but has not won one of the game's biggest titles since.
Augusta National co-founder and three-time Open champion Bobby Jones famously said that a player's career would not be complete without lifting the Claret Jug on the Old Course. And while McIlroy does not think that is strictly true, the world No2 was well aware of the significance of winning the oldest major title at the Home of Golf.
“I don't know if a golfer's career isn't complete if you don't, but I think it's the Holy Grail of our sport,” McIlroy said in his pre-tournament press conference on Tuesday.
Asked about the significance of winning after his round on Sunday, McIlroy told Sky Sports: “It would mean everything because of what I have been through the last few years, trying to get the fifth one.
“I have a lot of belief in myself, I know I can do it again. I just need to go out in my own little world and shoot a good score that I know I can do around here.”
Australia's Smith had been in pole position to achieve that feat after posting a record halfway total of 13-under par, but the world No6 three-putted the opening hole and made a double bogey on the 13th as he slipped off the pace.
Even an error-free front nine of 33 - with birdies on the fifth, sixth and ninth - had seen McIlroy a shot behind an inspired Hovland, who had birdied four holes in a row from the third to take over from Smith at the top of the leaderboard.
However, McIlroy then holed out from a bunker short of the 10th green for a stunning eagle to vault into the lead, before Hovland commendably held his nerve to birdie the same hole.
McIlroy found the green in two on the 614-yard 14th to set up another birdie and move into the outright lead, only to then fire his approach to the daunting 17th over the green and off the wall.
The resulting bogey dropped McIlroy back alongside Hovland, who brilliantly saved par from just over the green, with both players then making a birdie on the last.
Smith and Young will start the final round four shots behind after rounds of 73 and 71 respectively, with world No1 Scottie Scheffler and South Korea's Si Woo Kim a stroke further back.
Two-time Major winner Dustin Johnson is six shots back following a 71, with Tommy Fleetwood and US Open winner Matt Fitzpatrick on nine under with Australia's Adam Scott.
“Today when I was having breakfast it seemed everyone was making birdies everywhere," Fleetwood said after his 66. “I got a good start, the middle stretch was frustrating but a good finish again. The putts at 16, 17 [both to save par] and 18 feel crucial. I'd love to be in with a chance coming down the back nine tomorrow, but it is very special to still be in and amongst it.”
Additional reporting by PA.