A nanoscale spinel pillaring layer is introduced onto the surface of the LiNi0.8Co0.1Mn0.1O2 cathode material, which is confirmed by combined surface-probing techniques. The functional layer does not change the crystal structure after of pristine LiNi0.8Co0.1Mn0.2O2, while it plays a vital role in avoiding unfavorable side reactions occurred in the interphase between cathode materials and electrolyte. The treated sample shows suppressed capacity decay (19.3%) as compared to the pristine sample (41.9%) after 200 cycles at 2 C rate. Moreover, it can also improve the storage performance of LiNi0.8Co0.1Mn0.3O2 by restraining the generation of Li2CO3 and the NiO-like phase during the storage process in humid air. Thus, the capacity retention capability is improved after storage in air for 2 months, which improves from 52.2% to 77.6% after 200 cycles. Overall, this study offers an effective solution to improve the cyclability and storage stability of the Ni-based cathode materials.