After her discovery, she signed to Women Management in Milan, and later, VIVA in Paris in 2006. Her runway debut was at Just Cavalli for the spring-summer 2007 shows. She later walked for Paul Smith, Preen, and Marios Schwab in London. She made a comeback after not participating in fashion weeks at Milan and New York at the spring-summer 2008 Paris fashion week, walking for Balenciaga, Chanel, Dries van Noten, Miu Miu, and Louis Vuitton. In late 2008, she participated in the Victoria Secret Fashion Show 2008, in the PINK section. During the spring-summer 2009 season she walked over 35 runways for some of the world top designers, such as Chanel, Stella McCartney, Givenchy, Zac Posen.

Vilkeviciute has graced the pages of many fashion magazines around the world in including Vogue in Germany and France, Allure. In 2009, she appeared nude in a steamy photo shoot for Interview magazine with Zac Efron. She is the current face of Karl Lagerfeld, GAP in Japan, Dior Beauty and Emporio Armani. In the autumn-winter 2008 campaigns, Vilkeviciute replaced Hilary Rhoda as the face of clothing line Etro.