Tuning magnetic properties in layered magnets is an important route to realize novel phenomenon related to two-dimensional (2D) magnetism. Recently, tuning antiferromagnetic (AFM) properties through substitution and intercalation techniques have been widely studied in MPX3 compounds. Interesting phenomena, such as diverse AFM structures and even the signatures of ferrimagnetism, have been reported. However, long-range ferromagnetic (FM) ordering has remained elusive. In this work, we explored the magnetic properties of the previously unreported Cr-substituted NiPS3. We found that Cr substitution is extremely efficient in controlling spin orientation in NiPS3. Our study reveals a field-induced spin polarization in lightly (9%) Cr-substituted NiPS3, which is likely attributed to the attenuation of AFM interactions and magnetic anisotropy due to Cr doping. Our work provides a possible strategy to achieve FM phase in AFM MPX3, which could be useful for investigating 2D magnetism as well as potential device applications.
