It is their second win of the weekend together, having also won their foursome match on Friday morning at Whistling Straits.
Garcia made his debut at the 1999 Ryder Cup, appearing at nine further tournaments.
In 2006, he was unbeaten over the first two days, becoming only the second player after Ian Woosnam to win all four points from his foursomes and fourball matches.
Entering this year’s competition, Garcia had scored just as many points as the entire US team combined.
During the previous Ryder Cup at Le Golf National, France, in 2018, Garcia overtook Nick Faldo’s record to become Europe’s all-time leading points scorer with 25.5 points.
However, although he passed Faldo for the number of points, it took him until Saturday to pass him for the most matches won at the Ryder Cup.
Faldo had 23 matches won, but now Garcia is the record holder, having earned his 23rd and 24th match victories in Wisconsin.
When asked about breaking the record after his round, Garcia said it was “great,” although Europe’s predicament in the Ryder Cup was his sole focus.
When he was told about it on the 17th hole, he said he “didn’t know the record and I didn’t care.”
“It’s great but it’s not. We need more wins and unfortunately we are not getting them at the moment,” he told the media.
“Obviously Jon (Rahm) and I, we did what we had to and what we could, and unfortunately it just looks like the American guys are just playing a little bit better than us, and it’s a shame. But you know, we are not giving up. We’re going to fight until the end as hard as we can. Hopefully we have a good afternoon this afternoon and see what happens.”
Sergio Garcia becomes player with most matches won in Ryder Cup history