Layered transition metal dichalcogenides (TMDCs) host a plethora of interesting physical phenomena ranging from charge order to superconductivity. By introducing magnetic ions into 2H-NbS2, the material forms a family of magnetic intercalated TMDCs TxNbS2 (T = 3d transition metal). Recently, Fe 1/3+δ NbS2 has been found to possess intriguing resistance switching and magnetic memory effects coupled to the Néel temperature of TN ∼ 45 K [1,2]. We present comprehensive single crystal neutron diffraction measurements on under-intercalated (δ ∼ −0.01), stoichiometric, and over-intercalated (δ ∼ 0.01) samples. Magnetic defects are usually considered to suppress magnetic correlations and, concomitantly, transition temperatures. Instead, we observe highly tunable magnetic long-ranged states as the Fe concentration is varied from under-intercalated to over-intercalated, that is from Fe vacancies to Fe interstitials. The under-and over-intercalated samples reveal distinct antiferromagnetic stripe and zig-zag orders, associated with wave vectors k1 = (0.5, 0, 0) and k2 = (0.25, 0.5, 0), respectively. The stoichiometric sample shows two successive magnetic phase transitions for these two wave vectors with an unusual rise-and-fall feature in the intensities connected to k1. We ascribe this sensitive tunability to the competing next nearest neighbor exchange interactions and the oscillatory nature of the Ruderman-Kittel-Kasuya-Yosida (RKKY) mechanism. We discuss experimental observations that relate to the observed intriguing switching resistance behaviors. Our discovery of a magnetic defect tuning of the magnetic structure in bulk crystals Fe 1/3+δ NbS2 provides a possible new avenue to implement controllable antiferromagnetic spintronic devices.