We report a simple, scalable approach to improve the interfacial characteristics and, thereby, the performance of commonly used polyolefin based battery separators. The nanoparticle-coated separators are synthesized by first plasma treating the membrane in oxygen to create surface anchoring groups followed by immersion into a dispersion of positively charged SiO 2 nanoparticles. The process leads to nanoparticles electrostatically adsorbed not only onto the exterior of the surface but also inside the pores of the membrane. The thickness and depth of the coatings can be fine-tuned by controlling the f-potential of the nanoparticles. The membranes show improved wetting to common battery electrolytes such as propylene carbonate. Cells based on the nanoparticle-coated membranes are operable even in a simple mixture of EC/PC. In contrast, an identical cell based on the pristine, untreated membrane fails to be charged even after addition of a surfactant to improve electrolyte wetting. When evaluated in a Li-ion cell using an EC/PC/DEC/VC electrolyte mixture, the nanoparticle-coated separator retains 92% of its charge capacity after 100 cycles compared to 80 and 77% for the plasma only treated and pristine membrane, respectively.The rapid emergence and popularity of portable electronics has motivated extensive research efforts to meet the ever increasing demands for mobile power sources in terms of energy storage capacity, form factor, weight, and lifetime with minimal safety risk and environmental impact. Currently, Li-ion rechargeable batteries are the benchmark of this technology and are the subject of intense research and development.1-3 Certain operational limitations of the Li-ion batteries are directly or indirectly related to the performance characteristics of the separator that is a key component of each electrochemical converter. 4 The separator is essentially a diaphragm, whose function is to prevent physical and electrical contact between the electrodes, while allowing ionic current flow. [5][6][7] Ideally, the separators for Li-ion batteries should be porous and thin but mechanically robust. In addition, they should exhibit chemical and dimensional stability, low thermal shrinkage, and good wetting to common liquid electrolytes. Microporous membranes based on polyethylene (PE) or polypropylene (PP), their blends, their copolymers and their laminates have found widespread application as separators for Li-ion batteries, since they adequately fulfill most of the requirements presented above. The main drawback of the polyolefin separators is their poor wetting to cyclic electrolytes with high dielectric constant such as ethylene carbonate (EC) and propylene carbonate (PC), an effect that results in increased internal resistance of the cells. Modifications of the polyolefin surface can improve the wetting characteristics of the separators but the chemistry is rather challenging and the performance depends critically on the nature and the grafting density of the functional groups. [8][9][10][11][12][13][14][15] ...