This study describes a straightforward process for creating the two-component nanocomposite Fe2O3 and CoFe2O4 (CFO) at several pH values, including 9, 10, and 11 (referred to as CFO_pH 9, CFO_pH 10, and CFO_pH 11). The properties of the CFO materials were also analyzed and evaluated in relation to pH values using methods such as X-ray diffraction and scanning electron microscope. The results indicated that the average particle size of the CFO material decreased from approximately 46 nm to 21 nm. Conversely, the Fe2O3 phase ratio in the CFO materials increased when the environmental pH was adjusted from 9 to 11. Upon reaching a charge capacity of more than 1000 mAh g−1 in the first cycle, the CFO nanocomposites were also shown to be appropriate for use as the anode electrodes in lithium-ion batteries (LIBs). The CFO_pH 10 electrode exhibited a noteworthy retention of its high reversible capacity of 731.7 mAh g−1 even after 50 cycles of charging and discharging. This indicates that CFO_pH 10 nanocomposite has a great potential to replace graphite as the anode material in LIBs.