Very large magnetoresistance discovered in single crystals of the ferromagnetic Fe-intercalated transition metal dichalcogenide, Fe0.28TaS2 was attributed to the deviation of the Fe concentration from commensurate values (x = 1/4 or 1/3), which caused magnetic moment misalignments. Here we report a study of FexTaS2 crystals with 0.23 ≤ x ≤ 0.35, demonstrating that crystallographic defects lead to spin disorder, which correlates with magneto-transport properties such as switching magnetic field HS, magnetoresistance MR, and even zero-field resistivity ρ0 and temperature coefficient A in ρ(T ) = ρ0 + AT 2 : The ordering temperature TC and Weiss temperature θW are maximized at the superstructure composition x = 1/4, while Hs, MR, ρ0, and A are minimum. Conversely, at a composition intermediate between the superstructure compositions x = 1/4 and 1/3, the corresponding magneto-transport properties reach local maxima.