Disclosed is a method for preparing a porous carbon structure, the method comprising the steps of: (a) mixing a carbon precursor, a pyrolytic template, which is pyrolyzed at the carbonization temperature of the carbon precursor or removed by post-treatment after the carbonization of the carbon precursor so as to form pores, and a solvent, to prepare a spray solution; and (b) subjecting the spray solution either to spray pyrolysis or to spray drying and then spray pyrolysis, so as to form a carbonized carbon structure, and then removing the template from the carbon structure. A mesoporous spherical carbon prepared according to the disclosed method may have a large specific surface area and a large pore volume through the control of the kind and concentration of template, and thus can be used in a wide range of applications, including catalysts, adsorbents, electrode materials, materials for separation and purification, and materials for storing hydrogen and drugs.