In a wild, 14-point final game, Sharapova saved four match points. But on the fifth she pushed an easy forehand long, and she was out of the tournament after two rounds for the second year in a row.
The 2004 champion was playing in her fourth event since rejoining the tour last month following shoulder surgery in October. She's ranked 60th but was seeded 24th because of past success at the All England Club.
Dulko, ranked 45th, matched her best showing at Wimbledon by reaching the third round. She had won a total of only three games in two previous matches against Sharapova, but the Argentine repeatedly took charge of rallies by hitting drop shots, while Sharapova struggled with her serve and forehand.
In men's play, No. 28-seeded Mardy Fish of the United States matched his best showing at Wimbledon by reaching the third round when he beat Janko Tipsarevic 6-4, 3-6, 6-1, 6-4. Fish next play No. 4 Novak Djokovic, who defeated Simon Greul 7-5, 6-1, 6-4.
American Taylor Dent double-faulted 21 times and lost to Daniel Gimeno-Traver in the completion of a first-round match suspended because of darkness, 7-5, 7-6 (6), 4-6, 6-7 (3), 6-4.
No. 16 Zheng Jie, a semifinalist as a wild card last year, lost to Daniela Hantuchova 6-3, 7-5. No. 10 Nadia Petrova, No. 14 Dominika Cibulkova and No. 26 Virginie Razzano won.
Sharapova and Dulko played the afternoon's first match on Centre Court in warm sunshine, and the new roof remained open for a third consecutive day. Dulko was almost flawless at the start, committing only four unforced errors in the first 11 games.
But with a 3-love lead in the second set, she began spraying her shots, and Sharapova took advantage to win seven consecutive games.
Sharapova then wobbled, double-faulting to lose serve and fall behind 2-1 in the final set. She double-faulted twice in a row and lost serve at love to fall behind to stay, 4-3.
With Dulko serving in the final game, Sharapova lost two challenges as she fell behind 40-15. Always at her best under pressure, Sharapova hit a booming return and a feathery drop shot to overcome the first two match points, and her return winner erased another.
But with a point for 5-all, Sharapova pushed a backhand into the net, and she made errors on the final two points as well.
Sharapova fell to 6-1 this year in three-set matches. She finished with nine double-faults and had at least one in every service game in the final set.
Marat Safin's final match at Wimbledon took place Tuesday on cozy Court 18, tucked in a corner of the All England Club, closer to the exit than to the court where trophies are handed out.
That was appropriate, because Safin always seemed to have one foot out the door at Wimbledon. Playing his final year on the tour, the mercurial Russian lost in the first round to American Jesse Levine, 6-2, 3-6, 7-6 (4), 6-4.
Safin smiled when asked how he felt to be done at Wimbledon.
"Relieved," he said.
The two-time Grand Slam champion and former No. 1 never really took to grass, although he came to accept it as a brief, necessary annoyance at the start of each summer.
His best Wimbledon run came last year, when he reached the semifinals before losing to Roger Federer. But he won only 16 of 26 matches at the All England Club, and could recall only two where he played well - against Goran Ivanisevic in a loss in 2001, and in a win over Novak Djokovic last year.
"That's it," he said. "Not much."
So while Levine's victory was an upset, it wasn't really a surprise - not to Safin, at least.
"I knew that he's a talented lefty, tough player, fast, has nothing to lose, going to go for it," Safin said. "This is the toughest ones."
Levine, a qualifier from Florida ranked 133rd, earned his first tour-level victory this year and his first win ever over a top-50 player.
"Marat's a great player, and I've watched him play growing up," said Levine, 21. "So it's a pretty surreal experience to be his last match at Wimbledon."
The upset gave U.S. men a 2-6 record on the second day of the tournament. The other winner was two-time Wimbledon runner-up Andy Roddick, who beat big-swinging Jeremy Chardy 6-3, 7-6 (3), 4-6, 6-3.
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