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The nickel-rich ternary-layered oxide LiNixCoyMn(1-x-y)O2 (NCM) cathode exhibits high reversible capacity and low cost; however, severe capacity fade and aggravated air degradation prohibit its widespread commercialization. Herein, the hydrophobic fluoroalkylsilane-modified NCM811 cathode materials are reported. To better understand the effects of electrochemical properties of lithium-ion batteries, a variety of characterization techniques and electrochemical methods are utilized to study the surface chemistry at the cathode/electrolyte interphase. The hydrophobic fluoroalkylsilanes-grafted NCM811 cathode materials suppress the formation of residual lithium even after 30 days in humid air. The fluoroalkylsilanes layer can also provide chemical stabilization to the NCM811 cathode materials by anchoring transition metals (TM) and suppressing TM dissolution during long immersion times in electrolytes. Moreover, the degree of improvement depends on the structure of the fluoroalkylsilanes, such as the number of F groups and the length of carbon chains. As a result, FAS17-modified NCM811 cathode materials after 30-day humid air exposure (humidity 70%) exhibit the greatest overall capacity retention of 74.2% after 200 charge/discharge cycles.