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Driving Barcelona to Toulouse May 8, then Costa Brava May 10, then Barcelona May 12

We're renting a car in Barcelona leaving for Toulose May 8 V Day in France. Looking for diversions on the way. Staying in center city Toulouse. Recommendations?

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To add variety, you could drive Barcelona - Toulouse through the mountains via the c16, n20, a66 roads, crossing into France at Bourg Madame. Great scenery on the way, but no must-see stopping points.
If you make an early start, you could detour to Montsegur (Cathar stronghold), but you need to allow 3 hours for that detour+visit, meaning a late arrival in Toulouse and less time in Toulouse proper.