The pursuit of high-energy Li-ion batteries calls for the development of high-capacity electrode materials, especially anode materials. Graphite is a commercial anode but exhibits a moderate capacity of ∼350 mA h g −1 . In comparison, metal oxides provide higher capacities due to the potential to undergo conversion or alloy reactions. In this work, we revisit a bismuth ferrite (BiFeO 3 ) anode and reveal its underestimated performance by simple optimization of binders and electrolytes. We discovered that with the use of sodium carboxymethyl cellulose binder and fluoroethylene carbonate additives, this anode demonstrates a much-improved performance compared to that in previous reports. Specifically, it offers a high capacity of ∼750 mA h g −1 , an excellent rate capability at 1000 mA g −1 , and a stable cycling performance for 1050 cycles. When paired with an LiCoO 2 cathode, the full cell also demonstrates a promising cell voltage and rate performance. This work may motivate other similar materials to be used as high-capacity and long-cycling anodes for Li-ion batteries.