Just north of Ovimbundu territory lived the Mbundu, the second largest ethnolinguistic category, whose language was Kimbundu. In 1988 they made up an estimated 25 percent of the Angolan population. In the sixteenth century, most of the groups that came to be known as Mbundu (a name apparently first applied by the neighboring Bakongo) lived well to the east of the coast in the plateau region (at a somewhat lower altitude than the Ovimbundu); a few groups in the far northeast lived at altitudes below 700 meters. In general, the outlines of the area occupied by the Mbundu had remained the same. The major exception was their expansion of this area to parts of the coast formerly occupied by Bakongo and others.

Although most of the boundaries of Mbundu territory remained fairly firm, the social and linguistic boundaries of the category had shifted, some of the peripheral groups having been variably influenced by neighboring groups and the groups close to the coast having been more strongly influenced by the Portuguese than were the more remote ones. Moreover, the subdivisions discernible for the sixteenth century (and perhaps earlier) also changed in response to a variety of social and linguistic influences in the colonial period. The Mbundu in general and the western Mbundu in particular, located as they were not far from Luanda, were susceptible to those influences for a longer time and in a more intense way than were other Angolan groups.

There were a number of Kimbundu dialects and groups. Two, each incorporating Portuguese terms, gradually became dominant, serving as lingua francas for many Mbundu. The western dialect was centered in Luanda, to which many Mbundu had migrated over the years. The people speaking it, largely urban, had come to call themselves Ambundu or Akwaluanda, thus distinguishing themselves from rural Mbundu. The eastern dialect, known as Ambakista, had its origins in the eighteenth century in a mixed Portuguese-Mbundu trading center at Ambaca near the western edge of the plateau region, but it spread in the nineteenth century through much of eastern Mbundu territory. Another Kimbundu-speaking group, the Dembos, were generally included in the Mbundu category. Living north of Luanda, they had also been strongly influenced by Kikongo speakers.

By the late 1960s, the Mbundu living in the cities, such as Luanda and Malanje, had adopted attributes of Portuguese lifestyle . Many had intermarried with Portuguese, which led to the creation of an entirely new class of mestišos. Those who received formal education and fully adopted Portuguese customs became assimilados.

The Mbundu were the MPLA's strongest supporters when the movement first formed in 1956. The MPLA's president, Agostinho Neto, was the son of a Mbundu Methodist pastor and a graduate of a Portuguese medical school. In the 1980s, the Mbundu were predominant in Luanda, Bengo, Cuanza Norte, Malanje, and northern Cuanza Sul provinces.

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