Large magnetic anisotropy energy and out‐of‐plane easy magnetization direction are beneficial for the application of 2D ferromagnetism. Although the robust room‐temperature ferromagnetism is reported in Co–N‐doped graphene [Nat. Commun. 2021, 12, 1854], its magnetic anisotropy and easy axis of magnetization are still unclear. Herein, the magnetic anisotropy of CoN4–graphene and CoN3–graphene is systematically studied. The CoN4–graphene has an in‐plane easy magnetization direction, while the easy magnetization direction of CoN3–graphene is out‐of‐plane. The magnetic anisotropy energy can be tuned by injecting charge or applying strain. Especially, for CoN3–graphene, both charge injection and tensile strain can tune the easy magnetization direction from out‐of‐plane to in‐plane. The tunable magnetic anisotropy may promote the application of Co–N‐doped graphene in spintronic devices.
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