She brought along husband Brad Pitt and their six children to hit the country's famed museums, and enjoy tasty Spanish food.
Jolie told reporters Thursday she loves "Madrid and Barcelona mainly for art and great food."
Co-star Johnny Depp says he's looking forward to seeing Pablo Picasso's iconic "Guernica" painting. He also has friends in Madrid.
"The Tourist" was nominated for the Golden Globe awards' best picture, best musical comedy actor and actress.
