A few years ago I took a trip there with a mate. We rode down to the border with France and Spain and then turned left and effectively rode the border. After most of the day along the border we hit a campsite, before turning south the next day. I think we took a day and a half around Bardenas then headed north west off-road to Lagrono. After that it was back up towards the ferry at Santander, by road initially (the old road rather than the motorway) then off road west of Bilbao.
I expect I still have the GPS routes on my computer somewhere.
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