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Detailed theoretical and experimental investigations on the electronic and magnetic properties of the Mn₂Co_1−xV_xAl Heusler compounds are presented. The magnetization vs. temperature measurements on the Mn₂Co_1−xV_xAl Heusler compounds show a decrease of the Curie temperature with V content, between 745 K (x = 0) and 671 K (x = 0.5). Ferrimagnetic near fully compensated behaviour with the saturation magnetization of 0.29 μ_B/f.u. has been obtained experimentally for Mn₂Co_0.5V_0.5Al alloy, in slight disagreement with Slater-Pauling rule. The electronic band structure calculations performed using the Korringa-Kohn-Rostoker (KKR) Green’s function method for the Mn₂Co_0.5V_0.5Al alloy show half-metallic almost compensated ferrimagnetic behaviour with total spin moment of 0.02 μ_B/f.u.. Accounting for the preferential site occupation determined by total energy calculations results an increase …