Layered compounds LiNi1/3Co1/3Mn1/3O2 have recently received much attention as they have been regarded as a promising cathode materials for industrial application. However, its fast energy density decay and poor rate performance which originate from structure disruption especially at high rate and high cut-off voltage limit its large-scale application. Here, a novel designed concept and facile method were firstly used to fabricate (PO4)3− polyanions doped layered LiNi1/3Co1/3Mn1/3O2 (LNMC-(PO4) 0.015-O1.94) structure, which could offer more stable high-voltage cycling performance and high rate capability. We attribute this improved performance to the robust Ptet-O covalence, which will stabilize the oxygen close-packed structure during repeated cycling. Moreover, our stepwise pre-cycling treatments could effectively restrain the formation of micro-cracks and non-crystallization defects, and significantly improve cyclic durability with high charge voltage of 4.7V. The LNMC-(PO4) 0.015-O1.94 electrode can still delivers capacity retention of 81% after 200 cycles at a current density of 300mAg−1. The preliminary results reported here manifest that this novel-designed LNMC-(PO4) 0.015-O1.94 material represents an attractive alternative to ultrafast-rate, long-life and high-voltage electrode material for lithium ion batteries.