The Midnight Cowboy actor is currently in Israel as part of a fact-finding trip with former Arkansas Governor Mike Huckabee.
According to PA, Voight explained that he would "love to see" Jolie join him for a sojourn to the country in the near future to experience his "affection for Israel and the Jewish people".
"That would be a nice thing before I go," he said.
Jolie has served as a UN Goodwill Ambassador for nearly a decade, having visited flood-ravaged Pakistan and refugee camps in Sri Lanka on behalf of the organisation.
Voight won a 'Best Actor' Oscar in 1978 for his performance as a paralysed Vietnam veteran in director Hal Ashby's Coming Home.