The present invention relates to a method for preparing a carbon nanotube-carbon nanofiber composite, and a carbon nanotube-carbon nanofiber composite prepared thereby. The subject matters of the present invention are a method for preparing a carbon nanotube-carbon nanofiber composite, and a carbon nanotube-carbon nanofiber composite prepared thereby, the method comprising: a first step of dissolving an alkali metal precursor in a solvent to prepare an alkali metal precursor solution; a second step of dissolving a carbon-containing polymer in the alkali metal precursor solution to prepare a spinning solution; a third step of electrospinning the spinning solution to prepare carbon-containing polymer nanofibers having surfaces to which the alkali metal precursor is bound; a fourth step of heat-treating the carbon-containing polymer nanofibers to prepare carbon nanofibers having surfaces to which the alkali metal precursor is bound; and a fifth step of heat-treating the carbon nanofibers while a carbon source is supplied, so that the alkali metal precursor is activated as an alkali metal nanocatalyst, and the carbon source is bound to the surfaces of the carbon nanofibers by the nanocatalyst, and crystallizes and grows into carbon nanotubes, thereby preparing carbon nanofibers having surfaces to which the carbon nanotubes are bound.
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