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Oviedo, Asturias, is the largest "O" city in Spain; its population is 214,883 and it is Spain's 23rd-largest city overall.
The one that comes to mind, though, is Oporto, Portugal. Oporto (Porto in Portuguese) is Portugal's second-largest city, and is internationally known for its main export, port wine.
The next-largest Portuguese city starting with "O" is Odivelas, in Lisboa province; Odivelas's population ranks 14th in the country, with 54,624 people.
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