A high cut-off voltage is pretty pivotal for the improvement of the energy density of cathode materials. Unfortunately, high-capacity Ni-rich cathode materials usually show serious capacity attenuation at high cut-off voltage. Herein, we propose a Li2SiO3-surface modification strategy to highly improve the cycle performance of the Ni-rich LiNi0.8Mn0.1Co0.1O2 material at high voltage. The capacity retention of the pristine and Li2SiO3-coated electrodes is 57.6 and 77.7%, respectively, at the cut-off voltage of 4.6 V after 50 cycles. Meanwhile, the problems of polarization and voltage reduction of LiNi0.8Mn0.1Co0.1O2 are also alleviated. Our results show that Li2SiO3-surface modification is a very effective strategy for improving the cycle stability of Ni-rich cathode materials and can be used for other high capacity electrode materials.