To give him his due, he has come close, with seven top-10 finishes. But in the eyes of many he is defined by two high-profile failures.
The first was as a 19-year-old at Carnoustie in 1999 when he was probably the hottest property in golf. He had turned professional just three months earlier, won the Irish Open in only his sixth European Tour outing and was considered a contender on the strength of his proven links abilities only to implode spectacularly. He shot two rounds of 89, finished dead last and was seen sobbing in the arms of his mother.
Seven years on, having won a host of other titles, the Spaniard arrived at Hoylake ranked ninth in the world and was being touted as a favourite for the 2006 crown. This time, he lived up to his billing, never more spectacularly than on the third day, when he carded a 65 that was a clear six shots better than Tiger Woods had managed.
The two would be paired together on the final day in a Transatlantic epic. Garcia felt he was ready to get one over Woods, a player with whom his relations had been notoriously frosty down the years, and he didn't mind who knew.
He should have been more careful, though, for Woods was fired up by Garcia's braggadocio, and made the Spaniard pay. With cold-eyed precision, he taught Garcia a lesson and beat him by seven shots.
Garcia's bright yellow outfit that day is remembered as one of the greatest fashion disasters golf has ever seen but his play was just as bad. And somehow that day seemed to dynamite the idea that he was a shoo-in to clinch a major at some point.
In the eight years that have passed since then, and as another generation of players has emerged, Garcia has slipped off the radar screen reserved for players who are automatic contenders every time they tee up.
But has this year marked his return to that privileged elite? Garcia dropped as low as 78th in the world rankings at the end of 2010, but at the end of 2013 he was back in the top 10. A string of solid results has consolidated that position, and his performance yesterday took him up a notch again. Suddenly, we were watching a man who could yet collect the Claret Jug he craves.
With wondrous timing, Garcia warmed up for yesterday's round by watching Seve The Movie, the recently-released film of the early years of a golf icon. When he began with a Seve-esque bogey-eagle-bogey sequence over the first three holes, it was tempting to think he had been watching too closely but what followed was much more the work of a man with a major on his mind.
Garcia's second-hole eagle was a slam-dunk 6-iron from 162 yards, almost exactly the same distance as his slam-dunk 9-iron at the same hole (and with a more helpful wind) in 2006. A fluke, of course, but sometimes these things can put snap into a round that will subsequently crackle and pop, and that's exactly what happened with Garcia.
There was a distinct impression that the presence of Rickie Fowler in his group was adding spark to his game. The presence of Luke Donald - tour nickname Plod - might not have had quite the same effect but he and Garcia have a close, if improbable, friendship, burnished by their successful Ryder Cup partnership, and he was clearly comfortable in his group.
With that lumpy start in the rear-view mirror, Garcia birdied the fifth and 10th holes. At that point, with Rory McIlroy just starting out, he held a share of the lead with the Northern Irishman at six-under-par.
A bad error at 14, where he donned waterproofs to protect himself from thorns after hitting his tee shot into a gorse bush, pegged Garcia back to five-under but he got that shot back at the last with another birdie.
As he holed out, the roar around the 18th green was one of the loudest of the day. As silly as some of what he did (and said) in 2006 might have been, they remember him fondly in these parts.
"Fortunately, at this championship they want me to do well every time I play," he said afterwards. "I feel it and it's great. I want to do my best and it would be nice to win it for them as well as myself. I've been grateful for being able to do some things for Europe in the Ryder Cup but it would be nice to win an Open Championship as well.
"I have always enjoyed these courses and enjoyed playing where you have to think outside the box. It is our only major in Europe and I grew up watching Seve play in it. It is a little bit extra special."
Garcia added: "I have a lot of good memories from this Championship and from Hoylake. It's great to be there but I need to shoot a good round tomorrow and make sure I keep myself in contention and then see what I can do on Sunday."
As he left the interview area, Woods was just arriving. The American had just scraped into the weekend, on the cut line with nothing to spare. Garcia is eight shots better than Woods at the tournament's halfway stage. He had the good grace not to make his delight too obvious.