Actually, I think Joe Versus the Volcano may be my second favorite. That's a really excellent film.
My #2 isn't set in stone like my #1, but it would probably be either Walkabout, Wings of Desire, Picnic at Hanging Rock, Notorious, or Before Sunrise. If I could include a series, the Up Series would be high as well (and that one's more in line with the style of my #1).
what would be your #2? :)