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Li4Ti5O12 (LTO) has received considerable interest as an alternate anode material for high power density batteries for large scale applications. However, LTO suffers from poor Li+ diffusivity and poor electronic conductivity, resulting in capacity loss and poor rate performance. Here we demonstrate a facile synthesis of LTO NPs using liquid-feed flame spray pyrolysis (LF-FSP) which provides high surface area (∼38 m2/g) spinel structure LTO NPs with average particle sizes (APSs) of 45 ± 0.3 nm. Pristine LTO-Li half-cells exhibit reversible capacity of 70 mAh/g at 10 C. In this study, we show that mixing LiAlO2 NPs (5 wt %) and Li6SiON polymer precursor (10 wt %) with pristine LTO via ball-milling and ultrasonication followed by tape casting enhances the LTO rate performance providing reversible capacity of ∼217 mAh/g at 5 C over 500 cycles. The Li6SiON polymer electrolyte is synthesized from rice hull ash (RHA), an agricultural waste, providing a green synthetic approach to electrode coating materials. CV and EIS studies indicate that adding the solid and polymer electrolytes reduces charge-transfer resistance and electrode polarization, enhancing both reversibility and the LTO Li+ diffusion coefficient from 4.6 × 10−14 to 2.7 × 10−12 cm2/s.