AbstractCarbon‐on‐carbon materials carry the potential to be a major disruptive technology in fields like energy storage and electronics. In the present work, hot filament chemical vapor deposition (HFCVD) is used to synthesize carbon nanowall (CNW) tetrapods coupled to nanocrystalline diamond in a 3D hybrid network form. The CNW/diamond phase proportion as well as the structural morphology can be easily adjusted by the CVD parameters, allowing a single‐step synthesis of CNW micro‐ and nanopillars or CNW/diamond 3D hybrid materials, in the powder form or as interconnected free‐standing specimens. Additionally, the direct incorporation of SnO2 catalyst particles during the one‐step CVD process is demonstrated. µ‐Raman and electron microscopy are used to understand the evolution of the morphological characteristics associated to the growth mechanism. The electrowettability behavior of the novel CNW/diamond hybrid material is demonstrated by electrochemical polarization studies. Such multifunctional carbon‐based hybrid 3D nanomaterials can find promising applications in advanced technologies such as energy storage.