Promising aqueous zinc metal batteries (AZMBs) continue to face significant challenges regarding zinc anode reversibility due to detrimental reactions including hydrogen evolution and corrosion. Herein, the d‐band center is used as an “intuitive descriptor” to compare the hydrogen evolution activity of zinc‐based transition bimetallic oxides (ZTBOs) of fourth‐period transition metal elements, and the advantages of ZnTi3O7 (ZTO) functional protective layer in inhibiting hydrogen evolution and extending the lifespan of the zinc anode are selectively identified. The ZTO exhibits a lower d‐band energy level, which affects the adsorption of active H* and exhibits lower hydrogen evolution reaction activity. At the same time, the dense ZTO protective layer provides suitable ion channels to promote the uniform distribution of zinc flux and achieve uniform Zn deposition. Thus, cells with Zn@ZTO anodes exhibit over 6000 h of cycling stability (1 mA cm−2) and a high coulombic efficiency of 99.9% within 1200 cycles. Moreover, when paired with a V6O13 cathode, the assembled full cell exhibits excellent lifespan, retaining 86.9% of its capacity after 5000 cycles at 10 A g−1. This work provides new strategies and insights for designing inorganic protective layers, addressing HER‐related challenges, and advancing the practicality of AZMBs.