Layered transition-metal dichalcogenides (TMDCs) host a plethora of interesting physical phenomena ranging from charge order to superconductivity. By introducing magnetic ions into (, Ta; , Se), the material forms a family of magnetic intercalated TMDCs ( transition metal). Recently, has been found to possess intriguing resistance switching and magnetic memory effects coupled to the Néel temperature of [Maniv et al., Nat. Phys. 17, 525 (2021); Sci. Adv. 7, eabd8452 (2021)]. We present comprehensive single crystal neutron diffraction measurements on underintercalated (), stoichiometric, and overintercalated () 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 underintercalated to overintercalated, that is, from Fe vacancies to Fe interstitials. The under- and overintercalated samples reveal distinct antiferromagnetic stripe and zigzag orders, associated with wave vectors and , 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 . We ascribe this sensitive tunability to the competing next-nearest neighbor exchange interactions and the oscillatory nature of the Ruderman-Kittel-Kasuya-Yosida 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 provides a possible new avenue to implement controllable antiferromagnetic spintronic devices.