In this paper, carbon coated Li5Cr9Ti4O24 is prepared by using cystine as carbon source, which results in the formation of carbon co-doped with nitrogen/sulfur (CNS) coating layer after pyrolysis. Compared with carbon free Li5Cr9Ti4O24, the resulting Li5Cr9Ti4O24@CNS exhibits enhanced lithium storage capability. Cycled at 500mAg−1, it can be found that carbon free Li5Cr9Ti4O24 can only deliver the reversible capacity of 97.8mAhg−1 with capacity retention of 80.7% after 200 cycles. In contrast, Li5Cr9Ti4O24@CNS can maintain the reversible lithium storage capacity of 111.4mAhg−1 with capacity retention of 91.9% after 200 cycles. This improvement is attributed to the introduction of nitrogen/sulfur dual-doped carbon coating layer, which significantly enhances the electronic/ionic conductivity and reduces the charge-transfer resistance of Li5Cr9Ti4O24. Hence, Li5Cr9Ti4O24@CNS may be a promising anode candidate for lithium-ion batteries.