Introduction In recently, applicability of secondary batteries such as Liion batteries has been realized as power sources for portable electronic devices, electric vehicles (xEVs) and stationary power systems [1]. Consequently, a strong need for the highly electrical performances of batteries due to increase in the capacity constituting a battery pack has grown. Among cell properties, cyclability and safety are the most critical issues for application. According to previous studies, cyclability could be affected by metal dissolution from cathode active material, lithium plating at low temperature or overcharge conditions, and properties of solid electrode interphase (SEI) [2-3]. Safety issues mainly results from internal or external short-circuit of batteries, caused by direct contact of cathode/anode, lithium dendrite penetration to separator, separator shrinks or meltdown, and so on [4]. At present investigation, we develop a composite additive (called TOC) comprising flouropolymer and clay particles. The TOC will form a continuous phase and simultaneously modify the anode surface. The effects of novel additives have been examined by SEM, electrochemical and safety analysis. Beyond the electrolyte additive and cell design, this research proposes another facile strategy via surface modification that provides excellent protection to improve the cyclability and safety in the meantime.