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Beach out at the Barceloneta.
Take a walk through Montjuic and enjoy the views of the city from up top. Check out the Montjuic fountains that light up at night (check calendar).
As lowside said, La Sagrada Familia is a must see. If you want to see more of Gaudi's works, check out La Pedrera and/or Casa Batllo. I also checked out Parc Guell and Palau Guell as well.
Take a walk down La Rambla and go through the Bari Gotic (Gothic Quarter) while you're there and the Barcelona Cathedral, which is also in the same area. The Palau de la Musica Catalana is also in the neighbourhood. The architecture there is amazing.
Fan of Barcelona FC? Go to Camp Nou and take the stadium tour and Hall of Fame.
Bored? Go hunt down the cat statue in the Raval neighbourhood.
And yes, definitely watch for pickpockets!
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