Papaloukas helped lead the Greek national team to a EuroBasket title, in 2005, as well as to a FIBA World Cup silver medal in 2006, while always coming off the bench of the Greek national team. He was elected to the All-Tournament Team in both competitions. Papaloukas took part in two Olympic tournaments, in 2004 and 2008, with Greece finishing in their personal all-time best fifth position on both occasions. In 2006, he was named the FIBA Europe Men's Player of the Year.