Several models have been proposed to explain the origin of a chromitite stringer located at the contact between the Mafic and Ultramafic Sequences in the Unki Mine area of the Shurugwi Subchamber of the Great Dyke, Zimbabwe. A petrographic and geochemical study of this chromitite stringer was undertaken with the aim of constraining its origin. Forty-three chromite compositions were obtained from the studied chromitite stringer, which is characterized by a chromium number between 59.9 and 62.8 and a magnesium number which ranges from 37.8 to 46.4. The chromites at the contact zone in the Unki Mine commonly contains inclusions of sulfides, orthopyroxene, plagioclase, and/or amphiboles. The chromites likely formed early in the crystallization history of the Mafic Sequence, as they are commonly partially rimmed by sulfides and they occur as inclusions in plagioclase crystals. Unlike chromites from underlying Ultramafic Sequence chromitite layers, chromites at the contact zone contain low Cr2O3 contents which range from 39.4 to 42.6 wt.%. Furthermore, these chromites are enriched in Fe compared to most Great Dyke chromitites, which is interpreted to be a consequence of subsolidus exchange of Mg into orthopyroxene and Fe into the chromite. The absence of zoning in the chromites at this contact zone, and their low Mn, Fe contents, is consistent with attainment of equilibrium because the altered chromites often contain Cr-bearing magnetite rims. Two possible models for the formation of this chromitite stringer are mixing of relatively primitive and evolved magmas (i.e., ultramafic and anorthositic magma), possibly of different oxygen fugacities, and chemical diffusion across the contact between the Mafic and the Ultramafic sequences which resulted in melting at and below this boundary. The latter would have caused preferential loss of orthopyroxene from the underlying P1 Pyroxenite Layer, accompanied by re-precipitation of chromite at this contact.