This paper presents a detailed study of the formation of chromium-based alloys, Cr–Ta–W + plasticizing additives (Nb and Zr) and Cr–Ta–Si, during milling of powder mixtures in a Fritsch (P-7) planetary mill under an Ar atmosphere. It is shown that, after milling for 18 h, all the components of the starting mixtures convert into a Cr-based BCC solid solution. The powders of chromium alloys obtained in this study are readily compacted by hot isostatic pressing (HIP) under conditions typical of the processing of powders of high-temperature nickel alloys. Heating of the powders and compacts leads to the decomposition of the supersaturated solid solution and the formation of two forms of the Cr2M Laves phase with cubic crystal lattices. The formation of a mixed-phase fine microstructure in the chromium alloys after HIP suggests that the materials studied here are potentially attractive as a base of next-generation chromium-based high-temperature alloys.