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Abstract Recently, layered transition metal thiophosphate MPX₃(M= transition metals,X= S or Se) have gained significant attention because of their rich magnetic, optical, and electronic properties. Specifically, the diverse magnetic structures and the robustness of magnetism in the two-dimensional (2D) limit have made them prominent candidates to study 2D magnetism. Numerous efforts such as substitutions and interlayer intercalations have been adopted to tune the magnetic properties of these materials, which has greatly deepened the understanding of the underlying mechanisms that govern the properties. In this work, we focus on modifying the magnetism of Ising-type antiferromagnet FePS₃using electrochemical lithium intercalation. Our work demonstrate the effectiveness of electrochemical intercalation as a controllable tool to modulating magnetism, including tuning magnetic ordering temperature and inducing low temperature spin-glass state, offering an approach for implementing this material into applications.