My second suggestion - where I've actually been!
Incidentally, I've started a thread for 'how to get there, where to stay'
Where to go, how to get there? which might be useful for planning trips. This suggestion actually comes with built-in travel suggestion!
The Pyrenees are interesting all over - flowery meadows in the spring, birds of prey, good variety of insects. The Spanish side seems to me to be a bit bleaker, because hotter in the summer than the French side; and I prefer the eastern end to the western (the foothills go right down to pretty undisturbed coast), but that's personal.
A great way to get about the eastern French Pyrenees is on the petit train jaune -
http://www.countrycousins.co.uk/yelltren.htm or
http://www.villafrench.com/whattodo.htm The railway travels high above deep valleys (see raptors from above) and every stop has something interesting to see and somewhere to stay.