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Abdel Baset al-Megrahi died at home after his health quickly deteriorated. "He has been suffering from cancer for a long time and God choose him," Khalid al-Magrahi told NBC.
"He was too sick to utter anything on his death bed," his brother Abdel Hakim told Reuters. "We want people to know he was innocent."
Al-Megrahi was convicted in 2001 of the bombing of Pan Am Flight 103 as it flew to New York from London. All 259 people aboard the airliner were killed and 11 others on the ground in the town of Lockerbie, Scotland, died from falling wreckage.
Scotland freed him in 2009 on compassionate grounds because he was suffering from advanced terminal prostate cancer and thought to have months to live.
His release angered many relatives of the victims, 189 of whom were American, and the Obama administration criticized the decision.
Many speculated that a backdoor deal had been cut between the former regime of Moammar Gadhafi and the British government. With the fall of the Gadhafi regime in 2011, many in the U.S. and U.K. called on the new Libyan leaders to extradite Megrahi to serve out the remainder of his prison term, something Libya's ruling National Transitional Council refused to do.