Barcelona is a premier destination, and you can spend a week there and have plenty to see and do. But if you have more time, you can take off from there to other points in Spain either on day trips, with Barcelona as your base, or on longer journeys to other parts of the country.
Considering Barcelona's location in the northeast of the country, it is most sensible to explore Catalonia from Barcelona, and that's what most tours from the city do. However, more and more tours are using Barcelona as the starting point for a tour of the rest of the country.
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The impressive mountain of Montserrat is so close to Barcelona that you can see it in half a day. Then there's the museum of Salvador Dali in Figueres, along with nearby cities such as Tarragona and Girona and the beach town of Sitges. You can also take wine tours from Barcelona, along with tours that focus on Spanish food and drinks. High-speed trains make these trips easy and fast. You can either take an organized tour or just hop on the train yourself to Girona, Figueres, or other close locations and make a day of it.
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This tour is an extension of the four-day tour of Spain from Madrid. A bus journey from Barcelona to Madrid, via Zaragoza and Lleida, is added to the original tour, which takes you from Madrid to Cordoba, Seville, Granada, and Toledo. If you choose to go via high-speed train to Madrid rather than by bus, you will not see Zaragoza and Lleida, but you will have free time in Madrid to explore a bit before you leave the next morning after breakfast. You'll stay the stay the night in Madrid and also end the tour in the city, but no guided visits take place in Madrid on either occasion. If you want to return to Barcelona, you should take the six-day tour of Spain from Barcelona.
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This grand tour of Spain starts with two nights in Barcelona, before visiting Madrid for a night, followed by a tour of Andalusia, where you will visit Cordoba, Seville (for two nights) and Granada. Then your tour will return to Madrid via Toledo. You'll have guided tours in every city, plus free time to check out what interests you in Barcelona, Madrid, and Seville. You'll take a high-speed train from Barcelona to Madrid and then an air-conditioned bus with a guide to Cordoba, Seville, Granada, and Toledo. (This trip ends in Madrid and does not make a full circle back to Barcelona.)
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If you're interested in a longer trip, it's a better idea to go to Madrid and then take a tour from there. Madrid's central location makes it perfect for travel to the whole of the country, and it is quick and easy to get there from Barcelona. Or you can make Madrid your base and travel to Barcelona and Valencia on a four-day tour. It's easy and quick to get to Madrid from Barcelona or vice versa via high-speed train or via the Madrid-Barcelona Air Shuttle.