Li-rich and Mn-based layered oxides are the most promising candidates for next-generation high energy density cathode materials. However, inherent problems including poor rate performance, continuous capacity degradation, and voltage fading hinder their commercial utilization. Herein, a lattice-and interfacial-modified Li 1.2 Mn 0.54 Co 0.13 Ni 0.13 O 2 with a pristinelayered bulk structure, Na-and S-doped transition phase, and epitaxially grown Na 2 Mn (SO 4 ) 2 (C2/c symmetry) layer were constructed by Na 2 S treatment. The monoclinic Na 2 Mn(SO 4 ) 2 not only acts as an interface protective layer, alleviating the harmful electrode−electrolyte reactions, but also promotes formation of oxygen vacancy in the layered structure, enhancing reversibility of oxygen redox. The Na and S surface lattice doping leads to enhanced Li + diffusion and alleviates the chance of oxygen release. With the positive effects provided by the stable interfacial layer and lattice modification, the modified cathodes with moderate Na 2 S treatment shows alleviated capacity and voltage decay and enhanced electrochemical kinetics. Especially, the washed cathode with 3 wt % Na 2 S treatment delivers a discharge specific capacity of 305 at 0.1 C and 219 mA h g −1 at 1 C, as well as 93.15% capacity retention and 88.20% voltage retention after 200 cycles at 1 C.