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Margot Robbie did not improvise any widely publicized lines in Barbie. The most famous improvised moment involving her character was actually performed by Ryan Gosling, who shouted "Sublime!" unscripted, causing Robbie to genuinely laugh. While the set encouraged spontaneity, Robbie's major contribution was defending scripted lines, such as the final line "I'm here to see my gynecologist," which she and director Greta Gerwig fought to keep in the film.
While a number of hilarious, unscripted moments made it into the film, the most widely reported and famous instance of improvisation was performed by her co-star, Ryan Gosling, not Margot Robbie herself.
The most famous improvised line from the set was not from Margot Robbie:
Regarding Margot Robbie's lines:
In summary, while the set fostered improvisation from the cast, the widely celebrated improvised line belongs to Ryan Gosling, and no notable, specific improvisation by Margot Robbie has been widely publicized.
While the user asked about Robbie, it's worth noting that other cast members like Kate McKinnon (who improvised the 'Department of Sanitation' line) also contributed to the improv, not just Gosling.
While Robbie didn't improvise lines, her genuine laughter at Gosling's improv (like the 'milkshake' line) sometimes made it into the final cut or bloopers, which is a form of unscripted performance.