It brought to at least 12 the number of 55 wanted Iraqis in custody or believed killed.
The highest-ranking official in the group is Muzahim Sa'b Hassan al-Tikriti, who headed Iraq's air defenses under Saddam. He was No. 10 on the U.S. list of the most wanted officials from Saddam's regime.
Gen. Zuhayr Talib Abd al-Sattar al-Naqib, the former head of the Directorate of Military Intelligence, surrendered to U.S. troops Wednesday, a senior Pentagon official said.
The directorate monitored the loyalty of Iraq's regular army, provided security at Iraqi military facilities and collected intelligence on military forces opposing Iraq. Naqib was No. 21 on the 55 most wanted list.
Also captured Wednesday was Muhammad Mahdi al-Salih, the former Iraqi trade minister and No. 48 on the most wanted list.
Naqib was a professional soldier who rose through the ranks of the Iraqi army, U.S. officials said. The military intelligence directorate he headed was separate from the Iraqi Mukhabarat, which gathered strategic intelligence and conducted covert operations aimed at maintaining government authority.
Also Wednesday, allied special operations troops captured a Mukhabarat officer formerly in charge of American operations, a senior U.S. official said.
Jim Wilkinson, director of strategic communications for U.S. Central Command in Doha, Qatar, identified the prisoner as Salim Said Khalaf al-Jumayli. He was not among the 55 most wanted.
Al-Jumayli is suspected of having knowledge of Iraqi intelligence activities in the United States, including names of people spying for Iraq, Wilkinson said in a statement.
He offered no details about how the Iraqi was captured but said there was one Iraqi casualty during the operation. No Americans were hurt, he said.
The 56-year-old Naqib told The Los Angeles Times in an interview before his surrender that he made no apologies for his involvement in Saddam's government. He also made it clear that he had not always agreed with the Iraqi leader. However, he had shared Saddam's Pan-Arabist ideas and had hoped that Iraq and its military could be the force for creating an Arab nation, the Times report said.
Since early March, the United States has expelled at least five Iraqi diplomats, possibly because they were suspected of spying. It has also requested other countries to throw out Iraqi diplomats on their soil.