The aim of this work is to investigate electronic structure, magnetic properties and electrical resistivity of Fe₂V_1−xTi_xAl Heusler alloys. Numerical calculations give a pseudogap at the Fermi level for the majority-spin band of Fe₂TiAl and a magnetic moment larger than 0.9 μ_B, whereas the ground state of Fe₂VAl is calculated as a nonmagnetic semimetal with a very low total density of states at the Fermi level. In our calculations the remaining alloys of the Fe₂V_1−xTi_xAl series are nonmagnetic for x<0.1 and weakly magnetic for 0.1<x≤1. The magnetic moment μ of the series of Fe₂V_1−xTi_xAl compounds scales with the number of valence electrons and fits well to the Slater–Pauling curve. We also present a study of the electronic transport properties and magnetic susceptibility. The resistivities ρ(T) of Fe₂VAl and Fe₂V_0.9Ti_0.1Al are large and exhibit a negative temperature coefficient dρ/dT of the resistivity between 2 and 300 K. Below 20 K, ρ(T) also shows an activated character. The magnetic susceptibility of Fe₂VAl and Fe₂V_0.9Ti_0.1Al shows a maximum at ~2 K which could reflect either the disorder effect or the hybridization gap, characteristic of Kondo insulators.