In the area of aqueous Zn-NixCoy batteries, the application of MOFs derivatives has greatly improved the battery capacity, but it is still far from their theoretical capacity (~372 mAh/g). One reason is that high-temperature annealing makes the internal structure of MOF collapse and agglomerate, which covers a large number of reactive sites resulting in the low capacity of the battery. Another reason is that the optimal ratio of cobalt/nickel is still not confirmed, which has important influences on the discharge platform and capacity of the batteries. Here, the NixCoy-MOFs in different ratios were deposited on the surface of carbon nanotube fibers (CNTFs) using cathodic electrochemical deposition methods. The NixCoy-MOFs were deposited in five Ni/Co ratios (Ni-MOFs, Ni0.7Co0.3-MOFs, Ni0.5Co0.5-MOFs, Ni0.3Co0.7-MOFs, and Co-MOFs). There were then converted into amorphous NixCoyOOH through in situ electrochemical oxidation (Ni-OOH, Ni0.7Co0.3-OOH, Ni0.5Co0.5-OOH, Ni0.3Co0.7-OOH, and Co-OOH). Ascribing to the sufficient reactive sites and optimal electronic structure, the material Ni0.7Co0.3-OOH reveals a large capacity of > 300 mAh/g at a current density of 1mA/cm2. The Zn//Ni0.7Co0.3-OOH battery also shows a high capacity of > 300 mAh/g with a discharge platform of > 1.8 V.