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The Oscar-winning actress and Chris reprise their roles as love interest Jane Foster and the titular superhero in the Marvel sequel and admits shooting was often delayed by their uncontrollable giggling.
During an interview on UK station BBC Radio 1, she told Breakfast Show host Nick Grimshaw: "Chris Hemsworth and I definitely had some real immature laughing fits, which was amazing at first and then after five takes, people start looking at their watches and not being amused at all. So that sounds really silly but actually it was the hardest thing."
The 32-year-old actress admits their banter become "embarrassing" and the only way she could compose herself was to avoid eye-contact with her co-star Chris, 30.
She mused: "As soon as you try, it's like that reverse psychology thing when you try and stop and it makes you laugh. You try things like looking at their ear instead of their eye because you know that on a certain one or word or something you're just going to lose it ... we figured it out in the end."
Natalie also confirmed she will leave America to live in Paris, France, next year with her choreographer husband Benjamin Millepied and their son Aleph and she is intrigued to see if her French accent will fare well the locals.
She explained: "My family, we are moving to Paris a year from now. Very excited. I'll definitely not lose my American voice. Yeah well, you know, we'll test it out. I'll try and learn an accent. I'll try and do my best Jean Seberg and see what the response is."
