The reigning US Open champion and two-time French Open finalist Dominique Thiem squandered a two-set lead and left Roland Garros.
The fourth-placed Austrian was defeated 4-6, 5-7, 6-3, 6-4, 6-4 by 68th-ranked Pablo Andujar in the first round.
It was the first time in eight Grand Slam appearances that Team had lost their first game.
Andujar also defeated Roger Federer in Geneva earlier this month. For the first time in his career, Anduhar returned to win after losing the first two sets.
Team fell to 11-9 in five-set matches.
The team lost the 2018 and 2019 finals to Rafael Nadal.
Earlier, Naomi Osaka overcame a number of mistakes to win on her return to the French Open, and then did something no one knew if she would do: She spoke briefly to the audience.
The three-time Grand Slam champion and former No. 1 Angelique Kerber has already left the French Open with a third consecutive loss in the first round.