Photographed by Mario Testino, the 27-year-old star of "Spider-Man" and "Marie Antoinette" smolders in a white Grecian-draped Givenchy by Riccardo Tisci gown, Swarovski earring, scarlet lips and piercing eyes reminiscent of starlets past.
And we don't know if we've ever seen Dunst as pretty as she is in the inside spread, where her classic Grace Kelly-esque makeup is combined with edgier wears like a shredded one-shoulder dress by Rodarte, crystal-covered jacket by Burberry, see-through top by Patricia Field and a headpiece by British bad boy designer Gareth Pugh.
Aside from the highly stylized shots in issue #64 -- now out on newsstands -- Dunst opens up about taking on meatier roles, her special relationship with Kate and Laura Mulleavy, the sisters behind Rodarte, and the iconic artist and Louis Vuitton collaborator Takashi Murakami.
"She inspires us to be more creative," Kate Mulleavy says of her friend and muse, whom she hosted a casual Christmas dinner with in LA's Koreatown.
"She has a magical quality that all the greats, like Mia Farrow, have had before. You fall in love with her as a real person. She is both a character actor and a leading lady, which is a rare combination."
"I know I'll be seen in a different light," she says. "This role is the most I can show of myself and I think it's the best work I've ever done, for sure."
The starlet -- and sometimes Miu Miu model -- is also trying her hand at producing and directing with "Bastard," a short film she hopes to enter into the Tribeca Film Festival.
While she wouldn't tell V much, she confided that the movie is about "a two thousand year old religious tale told in a modern way," that was shot in the desert, involves a baby and also stars Lukas Haas.
"I didn't want to shoot the desert in a desert-y was, but more in a Woody Allen way," she says. "And we took a lot of inspiration from Paris, Texas."
Hmmmm... sounds like we'll just have to wait and see that one.
"I was just so surprised by how kind and humble he was," Dunst says of Murakami, who is also a friend of their mutual pal, Marc Jacobs. "I usually think artists are complicated... but he giggles like a little kid and gets so excited."
Murakami was also clearly happy with his choice in Dunst.
"I thought to myself, 'This is an actress,'" he tells V. "The minute McG yelled 'Action!' her entire face would change. She would completely transform herself, from the actress Kirsten to the Akihabara Majokko Princess. I was truly astonished."
As for the actress's future plans, she wants to keep astonishing people with her work, instead of the party girl image she became known for in the blogosphere for a few years. ("Kirsten Drunkst," anyone?)
"I'm ambitious. I want to do great work and work with great directors and do great movies and produce great films," she says. "I have criteria for myself that are probably too hard to meet, but I'm going to try. I think people who say they're not ambitious and have gotten to a place of success are lying."
To read more of Dunst's interview and see her entire high fashion photo shoot, head over to Vmagazine and pick up the issue, on newsstands now.
Also keep clicking to see which controversial model from V's previous issue makes an encore performance in V64.