Layered Li1.2Mn0.56Ni0.16Co0.08−xAlxO2 (0 ≤ x ≤ 0.08) cathode materials were successfully synthesized by a sol-gel method. X-ray diffraction and the refinement data indicate that all materials have typical α-NaFeO2 structure with R-3m space group, and the a-axis has almost no change, but there is a slight decrease in the c lattice parameter as well as the cell volume. Scanning electron microscopy and high resolution transmission electron microscopy prove that all the samples have uniform particle size of about 200-300 nm and smooth surface. The energy-dispersive X-ray spectroscopy mapping shows that aluminum has been homogeneously doped in the Li1.2Mn0.56Ni0.16Co0.08O2 cathode material. The cyclic voltammetry and electrochemical impedance spectroscopy reveal that appropriate Al-doping contributes to the reversible lithium-ion insertion and extraction, and then reduces the electrochemical polarization and charge transfer resistance. Li1.2Mn0.56Ni0.16Co0.08−xAlxO2 (x = 0.05) shows the lowest charge transfer resistance and the highest lithium-ion diffusion coefficient among all the samples. The Li-rich electrodes with low-level Al doping shows a much higher discharge capacity than the pristine one, especially the Li1.2Mn0.56Ni0.16Co0.08−xAlxO2 (x = 0.05) sample, which exhibits greater rate capacity and better fast charge-discharge performance than the other samples. Li1.2Mn0.56Ni0.16Co0.08−xAlxO2 (x = 0.05) also exhibits higher discharge capacity than the pristine one at each cycle at 55°C. These results clearly indicate that the high rate capacity together with a good high rate cycling performance and high-temperature performance of the low-Co Li1.2Mn0.56Ni0.16Co0.08−xAlxO2 (x=0.05) is a promising alternative to next-generation lithium-ion batteries.