Don't overlook the Pyrenees when focusing on the journey eastward.
N260 is the classic route east-west but there are great routes throughout Pyrenees including some of the cross-border passes.
I think the eastern section of the N260 is less dramatic and busier. So veer west a little way.
Other routes:
Gorge du Verdon (F)
Grande Route Des Alps. (F)
Have a look at any of the famous cols used on the Tour de France
Ride magazine has a useful resource of routes throughout Europe
The Ardeches and Cevennes area a bit inland are beautiful.
A few attractions:
Bessalu Moto Museum - the branch near Lerida. Excellent museum. They have one in Barca too - smaller I think. I haven't visited this one.
Historic towns: Besalu, Carcasonne
Millau bridge
Canal du Midi
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