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A series of SnO-coated alpha-Fe solid-solution nanocapsules were fabricated by a modified arc-discharge technique from Fe(1-x)Sn(x) targets with x = 0, 2, 3, 4 and 5 at%. The core and shells change with changing Sn concentration (0, 2, 3, 4 and 5 at%) in the Fe(1-x)Sn(x) targets used in the preparation. An in-depth study of the complex permittivity and permeability reveals that the SnO-coated alpha-Fe solid-solution nanocapsules with 3 at% Sn exhibit excellent microwave-absorption properties among the present SnO-coated Fe solid-solution nanocapsules, due to a proper electromagnetic match in the microstructure, the strong natural resonance as well as dipolar polarization mechanisms.