LiNi0.6Mn0.4O2 deserves greater attention because of its high thermal and cyclic stability, coupled with low raw material and production costs. However, this material suffers from low reversible capacity and poor rate performance. Herein, we rationally design a high-performance cathode structure composed of a robust conductive protective layer, gradient Li+ ions conductive layer and stable bulk phase of LiNi0.6Mn0.4O2 through surface cobaltization, which not only boosts the reaction kinetics of the electrode but also suppresses particle cracking and mitigates surface structural degradation. As a result, a dramatically improved rate capacity (118.7 vs 53.5 mAh g-1 at 5 C) and impressive capacity retention after 300 cycles (90.4% in a full cell) at a high cutoff voltage (4.4 V) are obtained. Co-modified LiNi0.6Mn0.4O2 is promising to challenge LiNi0.6Co0.2Mn0.2O2's commercial position attributed to the accessible capacity, superior rate capacity, excellent cycle performance, good thermal stability and low cost.