The present invention relates to a preparation method of a crumpled graphene-carbon nanoparticle composite using a microwave plasma system, which has excellent crumpling resistance and a large specific surface area with low number of stacked layers; and to a crumpled graphene-carbon nanoparticle composite prepared therefrom. The crumpled graphene-carbon nanoparticle composite of the present invention has excellent thermal conductivity, electrical conductivity, and mechanical strength, and can be applied as a material for various fields such as electrochemical sensors, solar cells, large-capacity capacitors, etc. The preparation method of the present invention comprises the steps of: preparing a graphene oxide colloid solution by dispersing graphene oxide in a mixed solvent including an organic solvent and water; and droplet spraying the colloid solution and treating the solution with microwave plasma.
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