An opposite-polarity electrospray technique is developed to synthesize Mn3O4-graphene hybrid nanomaterial that shows high specific capacity, fast charging/discharging capability, and long cycle life for lithium storage. The approach offers nanoparticle size control and tunability, morphology control, versatility for the synthesis of different materials and hybrid structures from different precursors, and continuous-flow nanomanufacturing with the potential for full automation.