In order to employ Li-ion batteries (LIBs) in next-generation hybrid electric and/or plug-in hybrid electric vehicles (HEVs and PHEVs), LIBs must satisfy many requirements: electrodes with long lifetimes (fabricated from inexpensive environmentally benign materials), stability over a wide temperature range, high energy density, and high rate capability. Establishing long-term durability while operating at realistic temperatures (5000 charge-depleting cycles, 15 year calendar life, and a range from À46 8C to þ66 8C) for a battery that does not fail catastrophically remains a significant challenge. [1] Recently, surface modifications of electrode materials have been explored as viable paths to improve the performance of LIBs for vehicular applications.[2] The cycle life and safety issues have been largely satisfied for Li x MO 2 (M ¼ Co, Ni, Mn, etc.) cathodes by coating the active material particles with a metal oxide and/or metal phosphate. [2a,2b,3] For anode, state-of-the-art materials such as Si suffer from significant volume expansion/contraction during charge-discharge leading to rapid capacity fade.[4] Natural graphite (NG) is a realistic candidate anode, for vehicular applications, due to its high reversible capacity, low and flat potential relative to Li/Li þ , moderate volume change, and low cost.[5] In previous reports, the performance of NG was improved by surface modifications with mild oxidation, [6] coating with amorphous carbon,[5c] metal oxides (Al 2 O 3 , ZrO 2 ), [5a,7] and metal phosphate (AlPO 4 ).[5b] These efforts were performed in order to mitigate the solid electrolyte interphase (SEI) [8] that is formed on the NG surface by reductive decomposition of the electrolyte during initial charge-discharge especially at elevated temperatures. The decomposition of the SEI at elevated temperature ($80 8C) is exothermic and initiates thermal runaway. [9] In most previous reports films of metal oxides and metal phosphates have been deposited on powder electrode materials with 'sol-gel' wet-chemical methods.