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Kroes described herself as a "tomboy" in her youth, though in 2003, she applied to modeling agency Paparazzi Model Management in Holland when older. The agency sent her to New York City, and after being cast a few times by Victoria's Secret, they asked her to try out as an "angel." When she moved to New York from the Netherlands, she had never heard of the brand before.
Kroes has been featured on the covers of Time, Vogue, Harper's Bazaar, Seventeen, Elle, Marie Claire, Glamour, W, Avantgarde, Dazed & Confused, and Numéro. She also appears regularly in the Victoria's Secret catalog and walked the runway of the company's fashion show in 2005, 2006, 2008, 2009, and 2011. Kroes's campaigns include Gucci, Tommy Hilfiger, Versace, Valentino, Blumarine and Calvin Klein for both their 'White' label and their fragrance 'Eternity'. In 2005, Kroes was selected as "Model of The Year" on Vogue.com by readers. She was presented on the May 2007 cover of American Vogue as one of the "World's Next Top Models" next to Chanel Iman among others. Along with several of these models, she appeared in the 2008 Pirelli Calendar