The Arab-language news network is launching an English-language international channel in the spring.
"Most of the television I have done over the years has been aimed at British and American audiences," Frost said in a statement released by al-Jazeera. "This time, while our target is still Britain and America, the excitement is that it is also the 6 billion other inhabitants of the globe."
The network noted that Frost has interviewed the last seven U.S. presidents and last six British prime ministers. In recent years, Frost has been the host of "Breakfast with Frost" on the BBC, which stopped airing in May.
Al-Jazeera has also recruited Josh Rushing, who as a military press officer appeared in the documentary "The Control Room." Rushing resigned from the Marines when he was ordered to stop responding to press questions after the documentary's release.