The stretched supply and high cost of cobalt harm commercial Lithium-ion batteries production and manufacturing, and the fundamental understanding of the influences of Co percent on the structure and electrochemical performance of LiNixMnyCo1-x-yO2 cathodes is lacking. Therefore, hydrothermal and high-temperature solid-phase methods prepared the LiNixMnyCo1-x-yO2 cathodes with different Co content. The basic properties of materials, such as crystal structure and overall morphology, are studied in detail using common XRD diffraction and scanning electron microscopy techniques. Meanwhile, the electrochemical performance was tested by a battery-testing workstation. For different Co content, all LiNixMnyCo1-x-yO2 cathodes present an intact layered structure with R-3m space group and exhibit acceptable reversible discharge specific capacities. The cathodes deliver higher initial discharge-specific capacity when the Co content is 0.08. The LiNi0.92Co0.08Mn0.1O2 presents higher discharge capacities of 191.8, 182.6, 167.3, 157.9, 143.8, and 116.6 mAh g−1 at different rates from 0.2 to 10 C, respectively. The electrochemical performance analysis results indicate that the LiNi0.92Co0.08Mn0.1O2 cathode exhibits better rate capacities and cycle performance before the 200 cycles.