Ivanovic, a former French Open Champion and world number one, lost 6-3 6-4 to become the second-highest seed to exit the women's draw after Simona Halep was beaten on Tuesday.
While it is seven years since the Serb clinched the title at Roland Garros, she had appeared to be on her way back to her best after reaching the last four on the Paris clay a month ago.
Yet she was put under pressure from the start by the tattooed American Mattek-Sands, who was playing in the second round at Wimbledon for only the third time.
"She was aggressive. She was coming in a lot. I thought she was hitting lots of winners off the forehand side," said the Serb whose boyfriend, Germany soccer international Bastian Schweinsteiger, was cheering her on in the crowd.
"She made some errors, but there was not really a rhythm out there, for example, like I had in my first match. I kind of expected that. She played well. She served well."
Ivanovic's career has been somewhat turbulent after she won the French as a 20-year-old in 2008.
Soon after that success, the results dried up as injuries and emotional instability on court took their toll, with her ranking dropping as low as 65 in 2010.
On the back of her Wimbledon exit, however, she said she will now take some time off to try and improve her fitness levels before returning to court in August.
"I'm looking forward to having some time off and do proper preparation because that's what I've been lacking," she said.
"I've been playing catch-up in that area for a while. I have lots of changes within the team. Now I feel like I have a solid base. But I just need time to first rest, refresh, and then work hard for it."
(Reporting by Toby Davis; editing by Ken Ferris)
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