High-voltage LiNi0.5Mn1.5O4 cathode material has gradually been one of the research hotspots. In this study, LiNi0.5Mn1.5O4 was prepared via a facile polymeric gel route. Compared with conventional sol-gel method, polymer network gel route can greatly improve the synthesis efficiency. The microstructure of as-synthesized LiNi0.5Mn1.5O4 was octahedron with uniform distribution. It proved an excellent electrochemical performance. The discharge capacities of as-synthesized LiNi0.5Mn1.5O4 were 132.2, 116.2, 102.5 and 82.3 mAh·g−1 at rates of 0.2, 2.0, 5.0 and 10 C, respectively. Over 60 cycles, the rate was restored to 0.2 C again, the discharge capacity (129.2 mAh·g−1) retention rate was 97.7% of initial capacity. The study we have performed showed that polymeric gel route was a facile powder technology to prepare high-performance LiNi0.5Mn1.5O4 cathode material.