Aqueous zinc‐ion batteries (AZIBs) suffer from rampant Zn dendrites growth, corrosion and sluggish transport kinetics, all of which have a serious impact on their performance and practical applications. Therefore, porous carbon nanofibers (BTO@PCNFs) loaded with BaTiO3 nanoparticles (BTO NPs) are constructed as a multifunctional interlayer for stabilizing the Zn anodes. Owing to the synergistic effect of BTO NPs and 3D porous carbon framework, this interlayer can achieve uniform electric field distribution, accelerate Zn2+ migration, and promote ion flux homogenization, thus leading to uniform Zn deposition. Meanwhile, the BTO@PCNFs interlayer demonstrates excellent anti‐corrosion effect, which can effectively prevent the side reactions. Benefiting from the synergistic effect of interlayers, the BTO@PCNFs multifunctional interlayers achieve a comprehensive optimization of the Zn anodes. The BTO@PCNFs‐Zn electrode exhibits lower nucleation overpotential (33.5 mV) at 0.5 mA cm−2. The Zn//Zn symmetrical cell with BTO@PCNFs interlayer exhibits ultra‐low overpotential (14 mV) and ultra‐long cycle life (5250 h at 0.5 mA cm−2). Even at high current density (30 mA cm−2), the BTO@PCNFs‐Zn electrode can be stably cycled for more than 830 h, achieving an ultra‐high cumulative capacity of 12 450 mAh cm−2. The multifunctional interlayers can provide a reference for the design of high‐performance Zn anodes.