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(Ti,V)2AlC solid solutions with Al2O3 addition were produced by solid state combustion involving aluminothermic reduction in the mode of self-propagating high-temperature synthesis (SHS). Starting materials included Ti/V2O5/Al/Al4C3 and TiO2/V2O5/Al/Al4C3 powder mixtures. Attempts were made to obtain (Ti1-xVx)2AlC with a broad substitution percentage. Combustion exothermicity was increased by increasing V2O5 for the yield of a higher proportion of V at the substitution site, which not only increased the combustion temperature and reaction front velocity, but also facilitated the evolution of (Ti,V)2AlC. The Ti-containing samples showed higher reaction exothermicity and better product formation than those adopting TiO2. As a result, (Ti1-xVx)2AlC with x from 0.2 to 0.8 was produced from the samples composed of the Ti/V2O5/Al/Al4C3 mixture. The (Ti,V)2AlC/Al2O3 composites synthesized in this study exhibited a laminated microstructure with closely-stacked (Ti,V)2AlC slabs of about 0.30.8 μm.