The performances of porous graphitic foams in flexible electronic, electrochemical, and thermal management devices can be enhanced by increasing the interfacial charge or heat transport between the 3D graphitic network and the functional materials filled into the pore space. Herein, an investigation of the effects of chemical vapor deposition (CVD) conditions on the structure and thermal conductivities of both graphitic foams grown from reticular Ni foams and dendritic graphitic foams (DGFs) synthesized from electrodeposited dendritic Ni foams is reported. A room‐temperature solid thermal conductivity () up to 800 W m−1 K−1 is obtained from the graphitic foams (GF) with less than 1% volume fraction. In comparison, the DGFs, which provide a large increase of the specific surface area for enhanced interfacial heat transfer, achieve an effective thermal conductivity of 2.5 ± 0.2 W m−1 K−1 because of an enhanced volume fraction to about 5% despite a compromised around 200 W m−1 K−1 due to the increased defect density. Through systematical variations of the catalyst template morphology and CVD conditions, this work reveals the distinct roles of catalyst surface curvature and graphitic strut thickness in controlling the properties of GFs and DGFs for thermal management.
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