Hi
I have a brother living in Pau and we rode from there throught the Pyreneese via Tarbes, Bagneres du Luchon, Arres to LLavorsi (HUMM 08).
This year we went via FOIX mainly motorway. The first route was better and pretty spectacular -despite all the roadworks. It should be in great condition now though.
As for going down through France, I did the motorways once :Loire, Bordeaux, to Biarritz and its long and not much fun on the motorway so I'd recommend staying off them and taking the country roads (depending on time). France didn't get interesting for me until the Loire Valley
So it depends on your time and where you want to end up. I can recommend Biarritz and San Sabastian (NW Spain). According to my brother, any of the lesser routes over the Pyreneese are great for biking.
Enjoy
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