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The development of low‐cost and high‐performance iron (Fe)‐based anode materials is of great significance for rechargeable aqueous batteries. Herein, a FeS@Fe foam anode with crosslinked nanoflake array structure is fabricated. Being adopted as alkaline anode, FeS@Fe foam delivers enhanced areal capacity of 31.1 mAh cm−2 (at 50 mA cm−2), which is ≈1.5 times that of the‐state‐of‐the‐art literatures. The scaled‐up tests further reveal the higher capacity (800.7 mAh) and current density (1.25 A) with the area of 25 cm2. The FeS@Fe foam anode sustains intact after 270‐day cycles, demonstrating excellent durability. The assembled FeS//NiO single battery provides a superior areal energy density of 300.7 Wh m−2 at 500 W m−2. The reaction mechanism and electrode kinetics are revealed by combining in/ex situ techniques and DFT calculations. Experimental results and in/ex situ characterizations validate that excellent structural stability and high areal capacity are attributed to effective interface regulation and improved energy storage mechanism, respectively. This work pushes the advanced Fe‐based electrode to a superior level among these available alkaline solid‐state batteries. [ABSTRACT FROM AUTHOR]