Magnetic moments intercalated into layered transition metal dichalcogenides are an excellent system for investigating the rich physics associated with magnetic ordering in a strongly anisotropic, strong spin-orbit coupling environment. We examine electronic transport and magnetization in Fe0.28TaS2, a highly anisotropic ferromagnet with a Curie temperature TC∼68.8 K. We find anomalous Hall data confirming a dominance of spin-orbit coupling in the magnetotransport properties of this material, and a remarkably large field-perpendicular-to-plane magnetoresistance (MR) exceeding 60% at 2 K, much larger than the typical MR for bulk metals, and comparable to state-of-the-art giant MR in thin film heterostructures, and smaller only than colossal MR in Mn perovskites or high mobility semiconductors. Even within the FexTaS2 series, for the current x=0.28 single crystals the MR is nearly 100× higher than that found previously in the commensurate compound Fe0.25TaS2. After considering alternatives, we argue that the large MR arises from spin-disorder scattering in the strong spin-orbit coupling environment, and suggest that this can be a design principle for materials with large MR.