Rose-like zinc-aluminum hydrotalcite (ZnAl-LDH) was synthesized in an organic/water mixed solvent system by a simple hydrothermal method and applied to zinc-nickel secondary battery, and its electrochemical performance as a negative electrode active material was also studied. Rose-like ZnAl-LDH has the characteristic diffraction peaks of ZnAl-LDH. SEM and TEM results show that the rose-like ZnAl-LDH was assembled by LDH nanosheets with the center as the axis and inclined at certain angles to form a rose-like structure. Through cyclic voltammetry, EIS and galvanostatic charge and discharge tests, rose-like ZnAl-LDH is superior to the coprecipitation synthesized flake-like ZnAl-LDH in cycle stability and discharge capacity. The initial discharge specific capacity of rose-like ZnAl-LDH is 363.4 mAh g-1, after 1250 cycles, the specific discharge capacity was 366.848 mAh g-1, the average discharge specific capacity was 392.455 mAh g-1 during the entire charge/discharge process. The results show that the rose-like ZnAl-LDH is a promising material with good cycle stability and high specific discharge capacity for energy storage devices.