The evolution of the electronic structure and magnetic properties with Co substitution for Fe in the solid solution Fe1−xCoxGa3 was studied by means of electrical resistivity, magnetization, ab initio band structure calculations, and nuclear spin-lattice relaxation 1/T1 of the 69,71 Ga nuclei. Temperature dependencies of the electrical resistivity reveal that the evolution from the semiconducting to the metallic state in the Fe1−xCoxGa3 system occurs at 0.025 < x < 0.075. The 69,71 (1/T1) was studied as a function of temperature in a wide temperature range of 2−300 K for the concentrations x = 0.0, 0.5, and 1.0. In the parent semiconducting compound FeGa3, the temperature dependence of the 69 (1/T1) exhibits a huge maximum at about T ∼ 6 K indicating the existence of in-gap states. The opposite binary compound, CoGa3, demonstrates a metallic Korringa behavior with 1/T1 ∝ T . In Fe0.5Co0.5Ga3, the relaxation is strongly enhanced due to spin fluctuations and follows 1/T1 ∝ T 1/2 , which is a unique feature of weakly and nearly antiferromagnetic metals. This itinerant antiferromagnetic behavior contrasts with both magnetization measurements, showing localized magnetism with a relatively low effective moment of about 0.7 µB/f.u., and ab initio band structure calculations, where a ferromagnetic state with an ordered moment of 0.5 µB/f.u. is predicted. The results are discussed in terms of the interplay between the localized and itinerant magnetism including in-gap states and spin fluctuations.