The defending champion was stunned 6-2 6-2 by the Spaniard in the second round at Roland Garros in a match that lasted just an hour and four minutes.
It was an extremely disappointing performance from the 17-time grand slam champion, who was broken five times by world number 35 Muguruza.
Williams won just 55 per cent of points on her first serve, and the 32-year-old accepted she was well below-par in that area of her game.
“Well, I don’t think anything worked for me today. I don’t know anything that actually worked,” the world number one said.
“I just can’t serve. I mean, my serve hasn’t been good yet. I can’t say this whole tournament, because my tournament didn’t last long, but yeah, just in general.”
The American was full of praise for Muguruza, who set up a third-round clash with Anna Schmiedlova after the Slovakian beat Williams’ sister Venus in three sets.
“She plays really well, obviously,” Williams added. “I have actually never seen her play like this. Hopefully she can keep it up, keep her form up and continue to play like this.”
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