Six alloys based on Cr-10Ta-7Si (by at.%) with quaternary additions of 0.5Ag, 5Ti, 1Hf, 3Mo, 3Al, or 3Re (by at.%) substituted for Cr were produced by vacuum arc-melting. The microstructures of the alloys were found to predominantly consist of a eutectic mixture of an A2 Cr-based solid solution and a C14 Cr2Ta Laves phase along with proeutectic Cr2Ta dendrites. Microstructural macro- and micro-scale inhomogeneities were observed in all alloy ingots, which were attributed to the non-equilibrium arc-melting process. The measured lattice parameters of the constituent phases and the elemental partitioning behaviour between the phases have been correlated with the respective covalent atomic radii. The bulk hardnesses of the alloys, along with the hardness of individual phases, have also been reported.