We developed a novel composite structure of MoS2 and naturally derived carbon as anode materials for lithium-ion batteries by using microalgae as both source materials and templates for nitrogen-doped hollow carbon with three dimensional internal structures. The microalgae-derived carbon performed the roles as conducting matrix and template for vertically stacked MoS2 nanosheets. The electrochemical performance of microalgae-derived carbon-MoS2 composite materials evaluated in half-cell system against lithium metal electrode secured capacity of 300 mA h/g after 880 cycles at current density of 5 A/ g. We ascribe the excellent cycle performance to the unique structure of hollow spherical microalgae- derived carbon with rich inner structures and naturally doped nitrogen, which consequentially facilitate fast lithium ion transport. This kind of structuring strategy is advantageous in terms of utilizing naturally created structures of microbes with complexed inner organelles and trace of heteroatoms, not to mention in respect of producing value added material from biomass residues.