Although lithium nickel cobalt manganese layered oxides with a high nickel composition have gained great attention due to increased overall energy density for energy conversion/storage systems, poor interfacial stability is considered a critical bottleneck impeding its widespread adoption. We propose a new approach based on immobilizing the artificial cathode-electrolyte interphase layer, which effectively reduces undesired surface reactions, leading to high interfacial stability of cathode material. For installation of artificial cathode-electrolyte interphases, a sulfonate-based amphiphilic organic precursor, which effectively suppresses electrolyte decomposition, is synthesized and subjected to immobilization on cathode material via simple wet-coating, followed by heat treatment at low temperature. The sulfonate-based artificial cathode-electrolyte interphase layer is well-developed on the cathode surface, and the cell controlled by the sulfonate-immobilized cathode exhibits remarkable electrochemical performance, including a high average Coulombic efficiency (99.8%) and cycling retention (97.4%) compared with pristine cathode material. The spectroscopic analyses of the cycled cathode show that the sulfonate-based artificial cathode-electrolyte interphase layer effectively mitigates electrolyte decomposition on the cathode surface, resulting in decreased interfacial resistance between electrode and electrolyte.