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It was the first time the 2011 champion had gone out at such an early stage of the tournament in seven appearances and wrecked her hopes of a second straight Grand Slam final appearance after Australia in January.
Asked if the cold, rainy weather had contributed to her downfall, Li replied: "Lose is lose, I cannot find another thing (to blame)
"The weather didn't change anything -- for both of us it was the same."
As she did in the first round against Anabel Medina Garrigues, sixth-seeded Li got off to a strong start winning the first four games before the stocky American rallied to win the next four.
Mattek-Sands then promptly undid all her hard work with a poor service game at 5-5 and Li took full advantage to take the opening set.
With dark clouds hovering over Court 1, Mattek-Sands broke early in the second set to lead 4-1 before the rain came down to suspend play for one hour 45 minutes.
They made a brief reappearance for 10 minutes during which Li pulled back to 4-3 with her serve to come before they were sent scurrying for cover once again as the heavens opened.
Another 90 minutes transpired before further play was possible and on the resumption, Mattek-Sands levelled the set scores by winning the next two games.
That appeared to sap all the confidence out of Li and she meekly surrendered the deciding set as the rain started to fall once again.
In the third round Mattek-Sands will play Argentina's Paula Ormaechea who defeated Yaroslava Shvedova of Kazakhstan 6-4, 7-6 (8/6).
Shvedova was the player who ended Li's French Open reign last year with a 3-6, 6-2, 6-0 upset fourth round win.
For 28-year-old Mattek Sands, it was just the second time she had reached the third round at Roland Garros in seven appearances, the previous being in 2011.
There was some success for China with Zheng Jie defeating Melanie Oudin of the United States 6-3, 6-1 to set up a possible third round matchup against defending champion and second seed Maria Sharapova of Russia.
But then the third Chinese player in the women's draw, Peng Shuai, went down 6-4, 6-3 to seventh seed Petra Kvitova of the Czech Republic foiling her bid to reach the third round at Roland Garros for the third straight year.
French Open results on Thursday (x denotes seeded player):
Men:
Second round:
Novak Djokovic (SRB x1) bt Guido Pella (ARG) 6-2, 6-0, 6-2
Grigor Dimitrov (BUL x26) bt Lucas Pouille (FRA) 6-1, 7-6 (7/4), 6-1
Victor Hanescu (ROM) bt Dmitry Tursunov (RUS) 6-4, 6-6 - retired
Philipp Kohlschreiber (GER x16) bt Lu Yen-Hsun (TPE) - walkover
Fabio Fognini (ITA x27) bt Lukas Rosol (CZE) 6-2, 7-6 (7/3), 2-6, 6-1
Kei Nishikori (JPN x13) bt Grega Zemlja (SLO) 6-1, 5-7, 6-1, 6-4
Women:
Second round:
Bethanie Mattek-Sands (USA) bt Li Na (CHN x6) 5-7, 6-3, 6-2
Paula Ormaechea (ARG) bt Yaroslava Shvedova (KAZ x27) 6-4, 7-6 (8/6)
Victoria Azarenka (BLR x3) bt Annika Beck (GER) 6-4, 6-3
Petra Kvitova (CZE x7) bt Peng Shuai(CHN) 6-4, 6-3
Jamie Hampton (USA) bt Anna Karolna Schmiedlov (SVK) 7-5, 6-2
Jelena Jankovic (SRB x18) bt Garbie Muguruza (ESP) 6-3, 6-0
Samantha Stosur (AUS x9) bt Kristina Mladenovic (FRA) 6-4, 6-3
Marina Erakovic (NZL) bt Dominika Cibulkova (SVK x16) 6-2, 2-6, 6-4
Sloane Stephens (USA x17) bt Vania King (USA) 6-1, 6-3
Zheng Jie (CHN) bt Melanie Oudin (USA) 6-3, 6-1
