Christian missionary work in Angola and Mozambique during the colonial and postcolonial eras was shaped by a complex of factors related to religion, education, and politics. Missionaries’ networks of local support played an outstanding role in their humanitarian work, particularly in the 20th and 21st centuries. By the end of the 19th century, Catholic and Protestant missions had established themselves in Angola and Mozambique. Until 1974, Protestants had a tense relationship with the Portuguese authorities, as they were suspected of serving the political interests of some European countries against Portugal, and later of supporting African opposition to colonial domination. Unlike the Protestants, the Catholic Church enjoyed a close collaboration with the ruling regime. Under the Concordat and the Missionary Accord of 1940 and the Missionary Statute of 1941, which were agreed between the Vatican and Portugal, Catholic missions enjoyed a privileged position to the detriment of Protestants, whose activities were severely restricted. The years that followed the independences of Angola and Mozambique in 1975 were characterized by open hostility to religion, aggravated by the nationalization of missions’ assets and properties in both countries. Mission activities related to education and health became hard to carry out. With the civil wars in Angola and Mozambique, warfare and dislocation gave a new social role to the churches. Between the mid-1980s and 1990 the first signs of new policies emerged. While in Angola the relationship between church and state was marked by ambiguity and mistrust, cooperation and collaboration prevailed in Mozambique, where the 1980s saw a rapprochement and constructive dialogue between the two institutions. This was sealed by the roles both Protestants and Catholics played in the peace and democratization processes. The political opening that characterized the 1990s and 2000s brought significant changes for both countries including the presence in the public space of new churches, especially those of Pentecostal denominations. The new sociopolitical contexts in Angola and Mozambique between the late 20th and early 21st centuries shaped the new roles of the missions, which remain more focused on social, rather than political, activities.