Athens is a crazy but very cool city. You'll hate it if you don't like crowds, hustle and bustle, and getting lost, but I like those things (to some extent), so it was great.
I highly recommend going to Delphi, and checking out the ruins of the Oracle there. It may be the most beautiful place I've visited in Europe.
Be sure to travel around the Peloponnese peninsula as well, stopping to check out Olympia, Mycenae, and Epidauros. Also Patra and Corinth are worth a visit.
As for islands, I've visited: Aegina, Dokos and Hydra in the Saronics, and they were nice to see, especially Hydra; Mykonos in the Cyclades which is worth seeing even despite its reputation as a gay haven; and in the Dodocanese, Rhodos (Rhodes) which is a really cool place but might be a bit too far afield for you, and Patmos which was quaint and where John wrote Revelation.
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