The crystal structure, morphology, and galvanostatic cycling and rate performances of cobalt-substituted Li 2 MnSiO 4 /C compounds, Li 2 Mn 1−x Co x SiO 4 /C (x = 0.25, 0.5, and 0.75), were evaluated and compared with those of Li 2 MnSiO 4 /C and Li 2 CoSiO 4 /C. Li 2 Mn 1−x Co x SiO 4 /C (x = 0.25, 0.5, and 0.75) compositions comprising uniform nanosized primary particles and no impurities were successfully synthesized using a hydrothermal method, followed by carbon coating. In addition, Li 2 MnSiO 4 /C and Li 2 CoSiO 4 /C were synthesized for comparison. The synthesized Li 2 Mn 1−x Co x SiO 4 /C (x = 0.25, 0.5, and 0.75) were solid solutions and were identified using an orthorhombic unit cell with Pmn2 1 space group symmetry. Although the capacity fades for Li 2 Mn 1−x Co x SiO 4 /C were similar to those for Li 2 MnSiO 4 /C, the discharge capacity, average discharge voltage and rate capability of Li 2 MnSiO 4 / C improved when Co was substituted for Mn. Li 2 Mn 0.25 Co 0.75 SiO 4 /C exhibited the best electrochemical performance with first energy density of 659.7 Wh kg −1 which was greater than that of LiMn 2 O 4 (500 Wh kg −1) and LiNi 1/3 Co 1/3-Mn 1/3 O 2 (600 Wh kg −1). The good electrochemical performance of Li 2 Mn 0.25 Co 0.75 SiO 4 /C is attributed to its lower charge transfer resistance relative to that of Li 2 MnSiO 4 /C.