The Namalulu tsavorite (vanadian grossular up to 0.80 wt.% V2O3) deposit in northeastern Tanzania occurs in metasomatized graphitic gneiss overlain by a dolomitic marble unit. These rocks belong to the Neoproterozoic metamorphic Mozambique Belt. The graphitic gneiss is composed of quartz, V-bearing kyanite (up to 0.4 wt.% V2O3), V-bearing muscovite (up to 1.0 wt.% V2O3), V-bearing rutile (up to 1.9 wt.% V2O3), and graphite. This rock is affected by calcic metasomatism precipitating calcite and mobilizing the elements for tsavorite crystallization in quartz-calcite veins. The dolomitic marble unit hosts an anhydrite-gypsum-dolomite lens (lens I) and a calcite-scapolite-diopside-sulfides-graphite lens (lens II). This last unit is characterized by the presence of F-bearing minerals (tremolite, phlogopite, tainiolite, titanite), with up to 9.4 wt.% F for tainiolite, and Ba-bearing minerals (feldspar, phlogopite), with up to 7.5 wt.% BaO for feldspar. Lithium (up to 2.0 wt.% Li2O) and boron (up to 110 ppm) are also present in tainiolite, as well as in F-bearing tremolite. This is the first description of metamorphic tainiolite. The protoliths of the Namalulu rocks correspond to organic-rich black shales, pure and magnesian carbonates, and evaporites. They were presumably deposited in a marine coastal sabkha located at the eastern margin of the Congo-Kalahari cratons bounded by the Mozambique Ocean during early Neoproterozoic. Tsavorite formed in the Ca-metasomatized gneiss during amphibolite facies retrograde metamorphism at 5.6–6.7 kbar and 630 ± 30 °C.