Eva Green first burst onto the cinema scene as an oft-nude revolutionary in Bertolucci's The Dreamers, then cemented her pin-status as a Bond girl in Casino Royale. The Hollywood-sceptic tells Xan Brooks about the indignities of working in the theatre and why she needs to fall in love

Some years ago I called up a young actor in search of some supporting quotes for an article I was writing on Bernardo Bertolucci. At the time, the actor was still living with her parents in Paris and had just appeared (sometimes clothed, sometimes not) in the director's swooning 60s-set drama The Dreamers. The actor was understandably concerned with how this debut role would be received. She didn't want to wind up like Maria Schneider, who famously ran off the rails after working with Bertolucci on Last Tango in Paris. The actor's mother was scandalised; her agent disapproving. I remember hanging up the phone wondering if we would ever hear of Eva Green again.

Skip forward six years or so and those fears seem ludicrous. Green, 30 next birthday, strolls into a London production office trailing a career that is embroidered with both art-house ventures and bona-fide blockbusters. She's been Princess Sibylla in Ridley Scott's Kingdom of Heaven, an exotic witch in Northern Lights and what was surely the franchise's most complex and nuanced Bond girl (admittedly a case of big fish, small pond) in Casino Royale. But if she feels vindicated, she's not showing it. "It doesn't satisfy me completely, this job," she says. "I want to travel. Maybe I'll end up living in Norway, making cakes."

Green is now based in London and has been shuttled across town, still half asleep, to plug the DVD release of Cracks, a stylish, silly, oddly enjoyable boarding-school pot-boiler that marks the directing debut of Ridley Scott's daughter, Jordan. Green plays the pulchritudinous Miss G, her eyes glittering through thick mascara as she whips up all manner of hormonal storms in her teenaged charges. "She's a great teacher, quite modern, but also cuckoo, you know?" she explains. "Quite fragile. Very Blanche DuBois." Cracks, she adds, is a small film, but that's OK. "It was good for the soul. I feel sick if I have to do something for the money. I can't breathe. I'm not proud of myself."

One has the sense that she is still calibrating her career. There was a point, after Casino Royale, when she could have relocated to LA and become Hollywood's French temptress of choice. She decided this was not for her. "I was in LA last week for a meeting and I don't like it. I get knots in my stomach and have to walk around a museum to make myself feel better. It's a cruel place, very hierarchical. If you're in the middle, you're shit, and if you're at the bottom, you're nothing. The people have no idea about anything that doesn't come from Hollywood. Most of them have never heard of The White Ribbon or A Prophet, and the only film of mine they know is Bond, because it made lots of money. I'm the Bond girl. It's as though it's written on my forehead."

In recent years she has made a concerted attempt to take the road less travelled; to make smaller films like Cracks, or Franklyn or an upcoming biopic of photojournalist Robert Capa. "I need to fall in love with someone," she says, and then shakes herself. "Sorry – I mean fall in love with something. I need to wake myself up."

She was born in Paris, the daughter of actor Marlene Jobert, who made films with Godard and Louise Malle. She is also the niece of Marika Green, whose roles ran the gamut from Robert Bresson's Pickpocket to Emmanuelle. Her dad worked as a dentist, although even he had a role in Bresson's classic Au Hazard Balthazar, about a donkey that may just be the messiah.

"Ah," she says. "But he couldn't stand Bresson. My aunt was in Pickpocket and [Bresson] was looking for a guy and my aunt said, 'How about my brother? He's very good looking, take him'. And my dad said OK and then hated the whole experience. You can see it in the film. He has two scenes – he's sitting on a bench and he looks so bored. Bresson could be very precise, very specific and he was quite hard on my father. My father was like, 'I'm a dentist. I don't want to be an actor anyway. Why are you shouting at me?'."

By the time Green made her grand arrival, in 1980, her mother had similarly turned her back on the acting profession. Jobert "lost the desire", explains her daughter, and went off to write children's books instead. She had fallen out of love with acting and had come to see it as a stressful and untrustworthy. It is a opinion that Green can relate to herself.

The way she tells it, her hazardous debut role in The Dreamers was not so much a launchpad as a re-birth. By that point she was in her early 20s and had spent a few years acting on stage. "I was bored with the theatre," she says. "I wanted to stop acting. I didn't believe in anything. But I did a lot of auditions to get the role. You can't turn down a role like that. You don't say no to Bertolucci."

What was her problem with the theatre? "I was in this play and I didn't get on with the director and didn't like the play. It was very grotesque, you know? Too much make-up and wigs and I was playing, like, this coquette. I was on stage for most of the time apart from three minutes when I was allowed to go off and pee in a bucket. And for those three minutes I was sitting on a bucket, peeing and crying at the same time." She laughs at the indignity of it all. "Oh, it was terrible," she says. "It was a nightmare. I hated it so much."

Our time is almost up. Green recalls that her drama teacher always told her that she would secure her best roles when she was in her 30s and she thinks this make sense, because even as a teenager she played mature characters, "Mary Tudor or Cleopatra. I never liked being Juliet – the ingenue." On the other hand, she's not entirely sure she wants to keep this up. She would rather produce, adapt books for the screen, or maybe just travel for a spell and then settle down in a different country. Acting, she says, is a strange and exposing job. She is always questioning herself; always fearing that she doesn't measure up.

Green's mother feared that acting might destroy her. Her agent insisted that she was too "fragile" to survive making The Dreamers. And the woman herself talks at length about the knots in her stomach, the breathing difficulties, the weeping on the bucket. All of which serves to paint a portrait of the artist as delicate flower, poised to wilt at the first sign of trouble. No doubt this is genuinely how she sees herself. I'm just not sure it's borne out by the evidence of her career, or even the evidence in front of me. The words tell one story and Green tells another. She seems, if anything, an extremely smart, cool and self-possessed individual; competent bordering on the formidable. Maybe she'll stick with the acting game. Maybe she'll jack it in to bake cakes in Scandinavia. Either way, I suspect that she'll be fine.

Cracks is out on DVD through Optimum Releasing.