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Three‐dimensional (3D) networks of graphitic carbon are promising materials for energy storage and conversion devices because of their high electrical conductivity, which is promoted by the good interconnection between the carbon particles. However, it is still difficult to directly synthesize such carbon networks. Herein, we report the novel synthesis of 3D graphitic carbon networks through the pyrolysis of nanosized ZIF‐67 crystals. Interestingly, the unusual effect of downsizing the ZIF‐67 crystals and the incorporation of catalytic Co nanoparticles was the spontaneous formation of graphitic networks. The obtained graphitic carbon networks show excellent electrochemical performance for the insertion and extraction of potassium ions.