If you mean Narbonne and you are going twice the length of the Pyrenees, I'm guessing you want to do some serious climbing, including a few of the big TdF regulars. In my opinion, you really shouldn't miss the Port de Pailhere, just to the East of Ax les Thermes. The summit is exactly 2,000 metres, and the descent features some of the best, most tightly packed hairpins I have ever encountered. I drove it in the car and the sat nav absolutely lost its S**t, repeatedly us to "perform a u-turn when possible". I believe it has been done at least once in the TdF and was classified HC. All I can say is that it is an absolutely stunning road and I wish I'd had the chance to ride it on a bike.
I'm totally unfamiliar with Spain or any of the places you mentioned, so thanks for the input. If it comes together, I'd like take in some of Spainish Pyrenees, rest up at my uncles near Narbonne and head back to the ferry (Santander - Plymouth) skirting the French Pyrenees.
It's been a while since I put myself out there in unfamiliar territory, the other alternative would be to pootle around in Brittany for the 4th time.