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One of the world's great cities.

Casa Mila by Gaudi, Barcelona

I happened to find a travel website with marvelous resources on Antoni GaudÝ, including photos of his buildings in Barcelona:
The Instituto Cervantes has posted a very rich site in Spanish about Gaudi:
Antoni GaudÝ wasn't the only Barcelona architect of note!  This site also has material on the other modernist architects:
My own personal list of Antoni GaudÝ sites, not to be missed, include:
Casa Mila (La Pedrera).  Passeig de Gracia 92.  See photo.  Visit the roof.
Parc GŘell.  Allow plenty of time for a leisurely visit to this fantasy park.
Casa Vicens.  Carrer dels Carolines 24.  Even though you will not be able to enter the building, I strongly recommend a visit to Casa Vicens.  See the photo.
Casa Batllˇ.  Passeig de Gracia 43.  Mosaics and animal shapes.
La Sagrada Familia.   Fantastic but, my advice is a little idiosyncratic.  It is unfinished, so there is less to see inside than in most churches.  A visit inside takes a lot of time.  Much of what is fabulous about the church you can see from the outside, especially from the park across the street.  If you do visit the inside, give yourself a break, and take the small elevator up the tower, rather than climb the stairs.
Our strongest recommendation for Barcelona has nothing to do with GaudÝ:  take a guided tour of the Palau de la M˙sica Catalana, Carrer Amadeus Vives 1.  This rich building is filled with turn-of-the century detail, including mosaic tiles.  See the photos below.  The architect was Lluis DomŔnech.
Aside from these architectural gems, walk the gracious boulevards, not just the Ramblas, which can be crowded.
Allow time for a visit to Montju´c.  There, you should visit Fundaciˇ Joan Miro, Parc de Montju´c, dedicated to the work of the artist Joan Miro.
Also on Montju´c is Museu Nacional d'Art de Catalunya.  This museum is one of  kind.  It collects the actual interiors of historic Romanesque churches from all over Catalonia, and preserves them in one large museum.  A visit to the original churches would have required weeks of effort, but it was impossible to care for them all.  The other half of the museum is interesting, too, but the collection of Romanesque churches is one of the most impressive museums I have seen anywhere in the world.
Barrio Gotic and the adjoining Ribera are the two oldest districts.  This modernist city also has a beautiful and historic gothic quarter.  In these districts, see:
Gothic cathedrall, Plaša de la Catedral.  Take a few minutes to visit the cathedral, but it is not one of the great cathedrals of Europe.  Its setting is more impressive than the interior.  Visit the cloisters.
Basilica de Santa Maria del Mar.  This beautiful Gothic church is more impressive than the cathedral.  It is the favorite chuch among the locals for weddings and concerts.
Museu Picasso , Carrer Montcada 15.  There are Picasso museums all over Europe, including Barcelona.  This was not one of our favorites, possibly because of the explicitly sexual nature of most of the works on display when we made our visit.
Above all in these old quarters of the city, take time to walk and explore.
We did not have time to see it, but a famous contemporary building is:  Museu d'Art Contemporani de Barcelona (MACBA)   by Richard Meier.
If you are visiting more than one museum, look for ARTICKET.
The multiticket initiative was launched by six of Barcelonas most important art centres. For 15 EUR , this combined ticket gives admission to the Museu Nacional dArt de Catalunya (MNAC), the Museu dArt Contemporani de Barcelona (MACBA), the Fundaciˇ Joan Mirˇ, the Fundaciˇ Antoni TÓpies, the Centre de Cultura ContemporÓnia de Barcelona (CCCB) and the Centre Cultural Caixa de Catalunya, La Pedrera.  The multiticket is available at the desks of all of the above centres, from any branch of the Caixa de Catalunya and via the Tel-entrada telephone booking service (902 10 12 12).

Casa Vicens by Gaudi, Barcelona

Palau de la Musica

Palau de la Musica, interior