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Caritas Angola began its activities in 1957. Until 1969, it helped communities affected by conflicts between the colonial Portuguese army and nationalist rebels fighting for their independence. Communities also need help during the first outbreak of Ebola hemorrhagic fever.

In 1970, Caritas Angola began to operate as an autonomous organization of Caritas Portugal. It seeks above all to mitigate the consequences of armed conflict. It identifies the highest concentration of people displaced by the war, and seeks to raise awareness about them in urban communities. It uses its relationship with Caritas Internationalis and other organizations to distribute basic necessities in the most dangerous and isolated areas and provides medical care and moral support to those affected by the war.

It provides assistance in an impartial manner, without religious discrimination. Caritas Angola is the only organization that has managed to distribute goods by air to Jamba, the headquarters of UNITA (the National Union for the Total Independence of Angola), and to other remote provinces.

In 1983, Caritas Angola began to work more as an institution, after a restructuring process that gave rise to a national secretariat to manage its operations. Between 1994 and 1996, diocesan commissions were created.

Today, Caritas Angola has 19 diocesan Caritas, and works in the following areas: institutional capacity building, disaster prevention and fundraising, influencing business and public policy, health care (especially for HIV/AIDS and maternal and child health), literacy and vocational training, and agriculture (with priority given to rural areas).

Caritas Angola maintains relationships with other national and international organizations, including OXFAM, Fundación Fé e Cooperação (FEC), Catholic Relief Services (CRS), Caritas Spain, Caritas Germany, Misereor and Entreculturas.