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The March 30, 1981, attack on Reagan left Brady partially paralyzed due to brain damage. His family said in a statement he died Monday morning after a series of health issues at a retirement community in Alexandria, Virginia, where he had been living for the past year and a half.
Brady spent the rest of his life in a wheelchair after being shot, but he and his wife, Sarah, campaigned for a gun law that would be known as the "Brady bill." The law, which was passed in 1993, required a mandatory five-day waiting period for purchase of handguns and also background checks for would-be gun buyers.
"As a result, countless lives have been saved. In fact, there are few Americans in history who are as directly responsible for saving as many lives as Jim," said Dan Gross, president of the Brady Campaign to Prevent Gun Violence.
Reagan was two months into his presidency when John Hinckley Jr. drew a $29 handgun outside a Washington hotel and wounded the president, Brady, a Secret Service member and a Washington police officer.
Reagan and his police guards fully recovered but Brady - known for his jovial manner and fondly nicknamed "the Bear" - was critically wounded from the .22-caliber bullet that exploded into his forehead.
Brady's situation was so critical that one television network erroneously reported he had died. But Brady, who was 40 years old at the time, made a near-miraculous recovery and left the hospital after a series of major operations that November.
After grueling sessions with physical therapists who Brady called "physical terrorists," he regained some speaking ability and some vitality but nevertheless was left paralyzed.
"Jim was the personification of courage and perseverance," Reagan's widow, Nancy Reagan, said in a statement.
Brady was kept on the White House payroll and technically remained press secretary, in name if not the actual spokesman, until Reagan left office in 1989.
President Barack Obama called Brady "a legend at the White House for his warmth and professionalism" and said he left a remarkable legacy of service.
"Since 1993, the law that bears Jim's name has kept guns out of the hands of dangerous individuals. An untold number of people are alive today who otherwise wouldn't be, thanks to Jim," Obama said in a statement.
The White House press room was named in Brady's honor and he returned there in 2006 at a ceremony temporarily closing the room for renovations.
"He leaves the kind of legacy that ... certainly this press secretary and all future press secretaries will aspire to live up to," White House press secretary Josh Earnest said at a daily news briefing.
In the years after the shooting, Brady and his wife, daughter of a gun-carrying FBI agent, became familiar figures fighting against handgun violence. They established the Brady Center to Prevent Handgun Violence and he was given a Presidential Medal of Freedom by President Bill Clinton in 1996.
The five-day waiting period on handgun purchases expired in 1998 and was replaced by a requirement of a computerized criminal background check.
"Jim Brady's zest for life was apparent to all who knew him, and despite his injuries and the pain he endured every day, he used his humor, wit and charm to bring smiles to others and make the world a better place," the family statement said.
Brady was born in Centralia, Illinois, on Aug. 29, 1940, and graduated from the University of Illinois. He taught at Southern Illinois University and worked in public relations before going to Washington in 1973 to work in the Department of Housing and Urban Development, Office of Management and Budget and Defense Department.
He also worked as press secretary to then-Republican presidential candidate John Connally, a former Texas governor.
After Connally lost his bid for the presidential nomination in 1980, Brady joined Reagan's staff.