Transition metal dichalcogenides can modulate their physical properties by introducing foreign species between the transition metal dichalcogenide layers. For example, when magnetic atoms are inserted into TiS2, different magnetic behaviors have been reported depending on their concentration. However, the relationship between the ordered arrangement of magnetic atoms and magnetism has never been clarified fully. In this study, FexTiS2 single crystals with Fe concentration from 0.05 to 0.33 were prepared. The purpose of this study was to clarify the characteristics of the ordered arrangement structure of iron atoms by systematically examining it using a spherical aberration-corrected scanning transmission electron microscope (STEM) system. In addition, the relationship between the ordered arrangement and measured magnetism was clarified.