By this I just mean a couple whose relationship develops in a particularly inventive way, you know the kind of thing that makes you think, 'That's brilliant.'

My second favourite is probably Paul and Holly from 'Breakfast at Tiffany's,' but my ultimate fave is Nino and Amelie from 'Amelie'! =DD They're perfect together and they know it, but they only meet 5 minutes before the end of the film!

I like Keanu Reeves and Barbara Hershey in Tune In Tomorrow. I think that it was also released as Aunt Julia and the Scriptwriter.

cheers

lesley

NANOWRIMO 2007 - The Spoonmaker's Diamond

When shall we live if not now - Seneca

I know anime probably isn't what you're looking for, but Kanji and Ogiue from Genshiken have my vote. Their relationship is handled with so much emotional realism, awkwardness included, that you can't help but get sucked in.
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Screnzy '08: Ceres. It's a romantic comedy between two mad scientists in space.
NaNo 2007: The Dragon Herald. (It's really not much like it sounds like.) Failed pretty badly, blah. :-/
NaNo 2006: Jerusalem O'Kira, Blockade Runner. I WON!

Amelie and Nino were brilliant :) Harold and Maude (eponymous) were pretty original. And I liked Mr. and Mrs. Smith :)

Tom

I think therefore I am pretentious.

Hm.... How about Edward and Sandra from Big Fish? I love the way they just kind of fall in "love" at first sight and he knows he's going to marry her, even though he knows nothing about her, and then they really do fall in love.

And John and Alicia Nash, from A Beautiful Mind. They're just so beautiful together, and the way they really need each other is rare. And it's a TRUE story, too :D

I could name another five dozen or so, haha, but I don't want to bore you. Ha.

Ada

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Is it bad that I miss the old you?

It was utterly and completely predictable, which was, of course, the whole point of the film, but I always liked the two couples in DOWN WITH LOVE. It wasnt that they were going to get together, it was how it was done, and some of it was so witty and stylish as to forgive the plotholes you could drive a semi through.

And although it probably doesnt count, save in a weird way: Tyler and the Narrator in FIGHT CLUB, definitely one of the strangest romances to ever come out of Hollywood.

How about:

1. Christian Slater and Patricia Arquette in "True Romance"
2. Bud Cort and Ruth Gordon in "Harold and Maude"
3. Ugo Tognazzi & Michel Serrault in "La Cage aux Folles"
4. Barbara Stanwyck and Gary Cooper in "Ball of Fire"
5. William Powell and Myrna Loy in "The Thin Man"

Naneaux

"I will not be cheated... nor will I employ long years of repentance in exchange for moments of joy." - Lady Mary Wortley Montagu

My favorite love story is definitely Noodles and Max in Once Upon a Time in America. Not a traditional or even romantic love story, but clearly a love story.

Also going to have to throw in a vote for Scarlett and Rhett. Because timing kind of is everything.

AND Lucy and George in Room With a View.

And in books, the award definitely goes to Clare and Henry in The Time Traveler's Wife. Oh and Anne and Gilbert in the Anne series.

Joel and Clementine in Eternal Sunshine of the Spotless Mind!!! One of my favorite films.

Jessica and Roger Rabbit. Oh yes.

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NaNoWriMo '07: The Squabbles of Nearly But Not-Quite Scientists; winner!
FAWM '08: "The Fall of the Candy Gladiator and Other Tales"; winner!
SF '08: In planning...

Elizabeth Bennet and Mr. Darcy. Nuff said. :)