Chimoio resigned after his school days in the Order of Friars Minor Capuchin. On 9 December 1979, he received the Sacrament of Holy Orders. Pope John Paul II has appointed Francisco Chimoio Bishop of Pemba on 5 December 2000. The episcopal ordination took place on 25 February 2001. On February 22, 2003, Pope John Paul II appointed Archbishop of Maputo.
In September 2007, he blamed as part of the 33 - year anniversary of the independence of Mozambique, the European states, deliberately infected with AIDS to provide condoms to Africa to promote the colonization of the continent. Chimoio said: " Condoms are not sure because i know thatthere are two countries in Europe, They Are making condoms with the virus on purpose ."