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Quang's campaign, in which he exhorted followers to emulate the example of Mahatma Gandhi, saw widespread demonstrations against the government of President Ngô Đình Diệm which, due to the influence of both Diệm's elder brother, the Roman Catholic Archbishop of Huế, Pierre Martin Ngô Đình Thục, and Diệm's younger brother, Ngô Đình Nhu, mistreated and persecuted the Buddhist majority. The suppression of Buddhists' civil rights and violent crackdowns on demonstrations, along with the self-immolation of at least five Buddhist monks led to a military coup in which Diệm and Nhu were deposed on 1 November 1963 and assassinated the following day.
In his early days, Quang went to Ceylon to further his Buddhist studies. When he returned, he participated in anti-French activities, calling for the independence of Vietnam. In 1963, Vesak (the birthday of Gautama Buddha) fell on 8 May. The Buddhists of Huế had prepared celebrations for the occasion, including the display of the Buddhist flag. The government cited a rarely enforced regulation prohibiting the display of religious flags, banning it. This occurred despite the non-enforcement of the regulation on a Catholic event celebrating the fifth anniversary of Ngô Đình Thục as Archbishop of Huế less than a month earlier. The application of the law caused indignation among Buddhists on the eve of the most important religious festival of the year, since a week earlier Catholics had been allowed to display Vatican flags to celebrate the 25th anniversary of the appointment of Diệm's brother Thục as Archbishop of Huế. The celebrations had been bankrolled by Diệm's regime through a national committee which asked the population to donate money to Thục's jubilee. Buddhists complained that they had been forced to give a month's wages to pay for the celebration.
On Phật Đản, thousands of Buddhists defied the flag ban. Trí Quang addressed the crowd and exhorted them to rise up against Catholic discrimination against Buddhism. He called the Buddhists to congregate outside the government radio station in the evening for a rally. Tension increased throughout the day with demonstrators chanting and displaying anti-government slogans as the crowd grew. They expected to hear another speech from Thích Trí Quang, but the speech was withdrawn from broadcast by the government censor. The military were called in to disperse the discontented crowd and fired directly into the crowd, killing nine were killed and severely injuring four. Thích Trí Quang spent the night riding through the streets of Huế with a loudspeaker, accusing the government of firing on the demonstrators. He then called on them to attend a public mass funeral for the Huế victims scheduled for 10 May. Such an emotion-charged spectacle would have attracted thousands of spectators and placed pressure on Diệm's regime to grant reforms, so the government announced a curfew and put all armed personnel on duty around the clock to "prevent VC infiltration". A confrontation was averted when Thích Trí Quang persuaded the protesters to lay down their flags and slogans and observe the 9 pm curfew. On the following day, May 10, tensions increased as a crowd of around 6,000 Buddhists attended Tu Dam Pagoda for the funerals and a series of meetings. Thich Tri Quang called on Buddhists to use unarmed struggle and follow Gandhian principles, saying "Carry no weapons; be prepared to die ... follow Gandhi's policies".
Thich Tri Quang proclaimed a five-point "manifesto of the monks" that demanded freedom to fly the Buddhist flag, religious equality between Buddhists and Catholics, compensation for the victims' families, an end to arbitrary arrests, and punishment for the officials responsible. Quang urged the demonstrators to not allow the Việt Cộng to exploit the unrest and exhorted a strategy of passive resistance.
As the crisis deepened, however, he traveled to the capital of Saigon for negotiations and further protests after the self immolation of Thích Quảng Đức on 11 June. Prior to the 21 August raid on the Xá Lợi pagoda engineered by Nhu's secret police and special forces, he sought refuge at the U.S. Embassy in Saigon. He was accepted by U.S. Ambassador Henry Cabot Lodge, Jr., who refused to hand him to Nhu's forces after they had ransacked pagodas, fired on civilians and beaten monks and nuns. In Huế, thirty people died as they attempted to protect their pagodas from Nhu's men.
Following the coup on 1 November 1963, which removed Diệm and Nhu from power, it was reported that the military junta wanted Thích Trí Quang to be a part of the new cabinet, but the U.S. State Department recommended against this. After the 1964 coup by General Nguyễn Khánh, which deposed the Dương Văn Minh junta, Khánh had Captain Nguyễn Văn Nhung, the bodyguard of Minh and executioner of Diệm and Nhu, executed. This generated rumours that pro-Diệm politicians would be restored to power and prompted Quang to cancel a planned pilgrimage to India to organise further demonstrations. In 1966, demonstrations occurred when anti-Diệm General Nguyễn Chánh Thi, the commander of central Vietnam, was stripped of his position by Prime Minister Nguyễn Cao Kỳ. Kỳ had Quang arrested and placed him under house arrest in Saigon. When the communists overran South Vietnam in the fall of Saigon in April 1975, Quang was again placed under house arrest.