In O Tetraperatos ("The Cunning") with Kostas Chatzichristos he sang "In Piraeus, in Piraeus" by Giorgos Katsaros, and in the romantic comedy Tzeni-Tzeni he and Tzeni Karezi performed a song by Giannis Markopoulos.
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Recognizing his great talent, Theodorakis took Poulopoulos under his wing and arranged for him to sing three songs in a theatrical production by Nikos Kourkoulos and Tzeni Karezi of Iakovos Kambanellis's play "The Neighbourhood of Angels".
For the soundtrack of the 1959 film To nisi ton genneon she recorded a song by the subsequent Academy Award-winner Manos Hadjidakis "Min ton rotas ton ourano" (Do not ask the sky) later covered by Brenda Lee as "All Alone Am I".
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Her stage debut was in the Marika Kotopouli theatre in the French comedy, La belle Heléne, with Melina Mercouri and Vasilis Diamantopoulos.
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In 1967, during the filming of Kontserto gia polyvola, she met Kostas Kazakos, "the love of her life" as she continuously said, with whom she gave birth to her only child, Konstantinos Kazakos.
Zoe Laskari, along with Tzeni Karezi and Aliki Vougiouklaki, were considered the three greatest divas and the most commercially successful female stars of the Greek cinema.