Echoing earlier replies, all the road on the Spanish Pyrenees are great riding territory. Col du Tourmalet may well be the greatest piece of road in the world, but when I was there last year, low cloud had the visibility down to 30 yds and resulted in the most terrifying hour of riding I've ever done.
For a damn good stretch of 90+ sweepers to contrast with the twisties, aim for the road from Lerida/Lleida to the med coast - simply outstanding. Of for fast, twisty empty mountian passes, aim for the mountains inland from Valencia. Don't know the name of the mountains, but the Puerto de Villaroya (5,100 ft) is a classic. Whole are is a little isolated, though.
You'd have to try very hard to not enjoy it!
Robin.