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Recent developments in 2D magnetic materials have motivated the search for new van der Waals magnetic materials, especially Ising‐type magnets with strong magnetic anisotropy. Fe‐based MPX3 (M = transition metal, X = chalcogen) compounds such as FePS3 and FePSe3 both exhibit an Ising‐type magnetic order, but FePSe3 receives much less attention compared to FePS3. This work focuses on establishing the strategy to engineer magnetic anisotropy and exchange interactions in this less‐explored compound. Through chalcogen and metal substitutions, the magnetic anisotropy is found to be immune against S substitution for Se whereas tunable only with heavy Mn substitution for Fe. In particular, Mn substitution leads to a continuous rotation of magnetic moments from the out‐of‐plane direction toward the in‐plane. Furthermore, the magnetic ordering temperature displays non‐monotonic doping dependence for both chalcogen and metal substitutions but due to different mechanisms. These findings provide deeper insight into the Ising‐type magnetism in this important van der Waals material, shedding light on the study of other Ising‐type magnetic systems as well as discovering novel 2D magnets for potential applications in spintronics. [ABSTRACT FROM AUTHOR]