Odysseus tells Calypso that he wishes to return to Penelope because

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In Book Five, Zeus sends Hermes to tell Calypso to let Odysseus leave her island immediately because it is not ordained that he will die far away from his family and friends. Odysseus's fate decrees that he will return to his native land of Ithaca. Calypso is upset that Zeus...

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In Book Five, Zeus sends Hermes to tell Calypso to let Odysseus leave her island immediately because it is not ordained that he will die far away from his family and friends. Odysseus's fate decrees that he will return to his native land of Ithaca. Calypso is upset that Zeus is forcing her to allow Odysseus to leave but acquiesces and gives him the provisions needed to make the journey home. Before Odysseus begins constructing his raft and leaves Calypso's island, the beautiful nymph promises to make him ageless and immortal if he chooses to remain with her. Odysseus responds by telling Calypso that he realizes that her beauty surpasses every mortal's appearance and that life on the island would be fulfilling but he cannot bring himself to stay. Odysseus mentions that he still has a desire to experience the feeling of returning home and has a heart that is prepared to bear affliction. He reasons that he has already been through so many troubles that enduring more difficulties will not dissuade him from leaving. Essentially, Odysseus still desires to see his homeland and believes returning home will justify the troubles he has experienced since the Trojan War.

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You can find the answer to this question in Book V.  At that point in the story, Athena has gone to Zeus and asked him to make Calypso let Odysseus go.  Zeus agrees with Athena and orders Calypso to release Odysseus.  Calypso is angry, but has to obey.

But first, she asks Odysseus if he wouldn't rather stay with her and become immortal.  Odysseus tells her that he realizes it would be wonderful but he just can't do it.  The only reason he gives is that he wants to go home and can't think of anything else but going home.

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