Sri Lanka comprises three roughly north-south trending amphibolite- to granulite-facies lithotectonic complexes, from west to east the Highland Complex, the Wanni Complex, and the Vijayan Complex. These terranes were correlated with other East Gondwana continental terranes with similar lithologies forming at similar ages. The Wanni Complex and the Vijayan Complex have been interpreted as volcanic arc terranes brought together by a double-sided subduction. The Highland Complex represents the metamorphosed accretionary prism within the suture when the Wanni and Vijayan Complexes were juxtaposing against each other. In contrast to the Wanni and Highland Complexes, the Vijayan Complex has yielded only a few geochronological data with satisfactory precision. Previous studies suggested that the Vijayan Complex comprises ∼1100–924 Ma granitic gneisses, which were metamorphosed during ∼590–456 Ma. More recently, ∼772–617 Ma mafic intrusions have been identified. This study divides the Vijayan granitic gneisses and the associated melt products geochemically into a low-Nb series and a more primitive high-Nb series. Our SIMS U-Pb zircon data suggested that both series have protolith magmatic ages of ∼1062–935 Ma, and metamorphic ages of ∼580–521 Ma, which is consistent with previous work. However, some of the Vijayan granitic gneisses and granitic anatectic melt products at the Highland-Vijayan tectonic mixed zone preserve an additional Tonian-Cryogenian (∼820–630 Ma) age signal. This age signal suggested that felsic magmatism also occurred when mafic granulites were emplaced along the Highland-Vijayan boundary, which is broadly coeval with to the bimodal magmatism occurring along the Highland-Wanni boundary. This study also suggests that charnockitisation in the Vijayan Complex occurred at 562 ± 6 Ma during the Neoproterozoic regional metamorphism. The Tonian-Cryogenian signal preserved in the Highland-Vijayan tectonic mixed zone can also be found in the alkaline intrusion hosted by the Namuno Terrane and the Lurio Belt in Mozambique. This indicates a relationship between the Vijayan granitic gneisses and the Lurio foreland metagranitic basement, while the Namuno Terrane and the Lurio Belt are correlated with the Highland-Vijayan tectonic mixed zone. The ages and the isotope signatures of these granitic bodies further suggest a genetic relationship of these granitic bodies with various magmatic intrusions in East Antarctica.