For more adventurous stuff in the spanish pyrenees/pre-pyrenees: check out Mont-rebei, Peņa Montaņesa, Ordessa. On the French side (just) the routes on Pic du Midi d'Ossau are long, fairly adventurous and not stupidly loose.
None of these are in anyway obscure, but they are more or less only visited by french or spanish speaking climbers. You will need a full rack for most of the routes, but not all.