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During a holiday in Mallorca last year I found some excellent driving roads, even in the holiday rent-a-jaloppy. Several months later I found two of the roads on Youtube https://www.youtube.com/watch?v=y1LhUzL3qdU&t=152s

and following the series of Greatest European driving roads on Youtube I drove the C462 Catalonia earlier this year experiencing all weather seasons in one day as you climb to over 1600m, https://www.youtube.com/watch?v=stxoXE0-4zQ&t=254s.

There's lots of other great driving roads in the border area with Andora, just pick the ones with the most squiggles in the atlas!

and this one on Mallorca https://www.youtube.com/watch?v=0P2k9lRsWOw&t=229s

Discov8 wrote:the C462 Catalonia [...] There's lots of other great driving roads in the border area with Andora, just pick the ones with the most squiggles in the atlas!

I concur: I drove the C462, and other roads around La Seu D’Urgell and Andorra, this time last year. My bit of advice is that, while I'm glad to be able to say I've been to Andorra, getting in and out wasn't worth it from a driving point of view.

David

Near Andorra, pretty much any section of the N260. C13/C28 from Sort to Viella is great.

Would concur with David that Andorra isn't worth the hassle. You can also lose time at border checks since it isn't schengen. Cheap petrol though

Sort is worth a visit if you are ever back that way again..

As a resident of Catalunya I wouldn't bother much with Andorra either as you can get caught coming both in and out as the place is not in the EU (see the future?). The place is all dull grey slate.
The police/customs are entitled to pull you a certain distance from the frontier as well (50k?) and frequently do - plus many speed traps especially on the French side. The money saved by buying there can soon be wasted on a fine.
However northern Catalunya is exceptionally pretty and there are some beautiful towns such as Olot/Ponts with the former having volcanos! On the French side is Aix Les Thermes which has hot sulphur streams and a fantastic spa.
As a further advert for Catalunya there are some good driving roads and mostly very well surfaced - I've not seen so many MX5s in any other part of the peninsular - the food and wine/beer are also excellent especially in the winter and autumn.
For a taste of the real Catalunya visit Vilafrance del Penedes for the Saturday market - this is the HQ of the Cava business and a prosperous town with more modernist architechture than many other places.