If you wanted something more recent, Summer Wars might be a reasonably safe bet. My opinion of it has deteriorated somewhat since I first saw it, but it's an accessible film that I think has a fairly broad appeal.
I do agree that you should base your recommendations on who you're aiming for though. I've been doing an occasional film review show on youtube for the past while, in which one of my friends and I swap film reviews to try and educate each other about our particular interests (mine being anime, his being horror), and I've tried to strike a balance between films I think he'll like and films that I think are important to anime as a medium.
It's thrown up some interesting results; he was not as keen on Akira as I thought he might be, but he really liked Space Adventure Cobra. Strangely, Summer Wars is not a film I've suggested yet, so I might feed him that soon and see what happens.