The carbon black (CB) is modified successfully by the two-step modifications such as organo-chlorination and organo-sulfuration using the chemical reagents of thionyl chloride and ethanethiol continuously. The organosulfur groups of-C-SR and-COSR forming on the CB surface play the main role to improve the electrochemical performances, which is verified by electrochemical studies. For instance, after carrying out the charge-discharge 100 times, the organosulfur modified CB (MCB) shows the Li + ion storage capacity at 392 mAh/g, which is higher than CB showing at 176 mAh/g. Furthermore, the improvement storage capacity is attributed to the enhanced capacitive effects which are verified by the detailed measurements of cyclic voltammetry (CV). These results are able to provide effective way to enhance the storage capacity of general carbon materials such as CB, graphite, graphene oxide (GO) and so on.