flexibility, and operation safety are urgently required. [1] Nickel-zinc batteries using non-flammable aqueous electrolyte and low cost zinc anode are regarded as one potential candidate in flexible energy storage fields due to their high output voltage (about 1.7 V) and theoretical energy density (816 Wh kg −1 based on α-Ni(OH) 2 cathode and Zn anode), outstanding intrinsic safety and low production cost. [2] However, their large-scale application was hindered by low practical energy density and poor cycle performance owing to the poor electrical conductivity, retarded ionic diffusion kinetics and severe crystal structural collapse of the Ni-based cathode during cycling. [3,4] Therefore, high performance flexible Ni-Zn batteries requires the simultaneous realization of the ionic transport kinetics, mechanical flexibility and structural robustness of the electrodes even upon the high-rate cycling. [4] Nickel hydroxide has been widely used as the cathode of Ni-Zn batteries due to its high redox potential, high specific capacity, and easy processability. [5] The nickel hydroxide demonstrates a hexagonal layered structure with two forms of crystals, namely the α-Ni(OH) 2 and β-Ni(OH) 2 . [6][7][8] The α-Ni(OH) 2 exhibits a large interlayer distance of ≈0.7 nm due to anions and water molecules intercalation into the interlayer space, which thus guarantees the reversible phase transformation between the α-Ni(OH) 2 and γ-NiOOH during the charge/discharge process without obvious volume variation. [7,9] The oxidation state of nickel in γ-NiOOH is 3.3-3.7, thus the α-Ni(OH) 2 can demonstrate the largest reversible theoretical capacity of 480 mAh g −1 . In the sharp contrast, the β-Ni(OH) 2 can only reversibly convert into the β-NiOOH, and lead to serious structure damage and structural evolution into the γ-NiOOH due to the small interlayer distance of ≈0.46 nm for β-Ni(OH) 2 . [7] The oxidation state of nickel in β-NiOOH is only 2.9, thus the β-Ni(OH) 2 shows a reversible theoretical capacity of 286 mAh g −1 . However, the α-Ni(OH) 2 is unstable and can easily transformed into β-Ni(OH) 2 in the strong alkaline solution, let alone the retarded ionic/electronic conductivity, which limit the power output of the Ni-Zn batteries. [6] The introduction of heteroatoms such as Co, [10] Al, [11,12] Zn, [5] Y, [13] etc. for partially substituting Ni 2+ in α-Ni(OH) 2 was regarded as one efficient strategy to enhance the stability of α-Ni(OH) 2 in alkaline solution. The heteroatoms can stabilize the α-phase through anchoring the anions (CO 3 2− , NO 3 − , The α-Ni(OH) 2 is regarded as one promising cathode for aqueous nickel-zinc batteries due to its high theoretical capacity of ≈480 mAh g −1 , its practical deployment however suffers from the poor stability in strong alkaline solution, intrinsic low electrical conductivity as well as the retarded ionic diffusion. Herein, a 3D (three dimensional) macroporous α-Ni(OH) 2 nanosheets with Co doping is designed through a facile and easily scalable electroless plating combined with elect...