A low temperature method for incorporation of surface ions has been adopted for the lithium-excess layered cathode material Li[Li0.2Ni0.13Co0.13Mn0.54]O-2 with NH4BF4 as the modification compound. A complete and continuous modification layer is gradually formed during the entire electrochemical cycling process. The modification effectively prevents the formation of lattice imperfections on particle's surface region despite running for 50 cycles. The absence of the 530.5 eV peak at 2.0 V for the modified electrodes in the X-ray photoelectron spectroscopy analyses illustrate improved redox reversibility of oxygen, which contributes to the superficial stability of the structure. Enhanced electrochemical performance is achieved and the voltage decay is relieved from 202 mV to 65 mV after 55 cycles. The surface crystal structure is stabilized with the lengthened M-F and B-M bonds by the formation of strong B-F bonds due to the insertion of BF4-tetrahedron and the surface oxygen ions are stabled. (C) 2017 The Electrochemical Society. All rights reserved.