Extensive scale commercial application of zinc nickel battery is limited for its poor cycle stability. In this paper, a zinc anodic material with ultra-high cycle stability is explored by structural design and element doping of Zn-Al layered double oxides (Zn-Al LDO). Flower-like Zn-Al-In LDO and pure Zn-Al LDO are synthesized by facile hydrothermal and calcination methods. Compared with pure Zn-Al LDO,Flower-like structure provides more pores to promote the electrolyte penetration and effectively reduce the local current density. The indium additive with high hydrogen evolution overpotential in Zn-Al LDO inhibits the corrosion of zinc electrode in high concentration alkaline solution. After a series of electrochemical tests, Zn-Al-In LDO has the lowest redox voltage (0.448 V vs. Hg/HgO) and lower charge transfer resistance (1.053 Ω). Meanwhile, compared with pure Zn-Al LDO, the corrosion potential and corrosion current of Zn-Al-In LDO are significantly reduced to (−1.372 V) and (−0.01458 mA cm−2) and the capacity retention rate of flower-like Zn-Al-In LDO is always above 90% within 2000 cycles. The rational design of flower-like Zn-Al-In LDO microsphere electrode paves new ways to develop the high-performance of zinc-nickel secondary batteries.