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Spain, best travel route between Madrid & Barcelona?

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We will be in Spain In mid-November. Trying to figure out the most efficient route between Madrid and Barcelona. All modes are fine with us and we are comfortable with public transportation. My husband thinks flying would be the most efficient way. Counting the time getting to and from airports and flight time, is this really the better option?

What would be the benefit if we drove (interesting stops)? Or just rent a car in either city to travel a bit outside the city itself.

We also plan to visit Toledo and I see there are lots of postings here about that, as well as all manner of recommendations for visiting the two cities.

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