For a lot of visitors, La Laguna is the nicest city if you want charm, history, and an easy walk around town. If you want a holiday feel rather than a city break, Costa Adeje is usually the better choice, though it is more a resort area than a true city.
Puerto de la Cruz is also popular because it feels more local and less hard selling than the south. “Nicest” depends on what you mean, quiet streets, old buildings, beach access, or nightlife. For most people, La Laguna wins on character.
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