Carbonatite tephra was discharged in the final eruptive phase of Kerimasi, an extinct nephelinite volcano in the eastern rift valley of northern Tanzania. The tephra was dominantly of alkali carbonatite composition, thus providing the first well-documented example of premodern natrocarbonatite volcanism. The principal carbonate mineral was nyerereite, which is the dominant mineral in modern natrocarbonatite lava flows of the adjacent volcano Oldoinyo Lengai. The nyerereite of Kerimasi was leached of its alkalis by meteoric water and is now represented by calcite pseudomorphs. Natrocarbonatite tephra of Kerimasi shows that the alkali-rich eruptive rocks of Oldoinyo Lengai are not unique, thus supporting the hypothesis that carbonatite magmas associated with nephelinite volcanism were originally alkaline and that the subvolcanic calcitic carbonatites are a residuum from which the alkalis have been removed, either by volcanism or fenetizing fluids. A hypothesis to be tested is that eruptive carbonatite magma is, worldwide, commonly and perhaps dominantly of natrocarbonatite composition.