Given the specific properties of each carbon allotrope such as high electrical/thermal conductivity of multi wall carbon nanotubes (MWCNT), and extreme hardness and high inertness of nano-crystalline diamond (NCD), the integration of both carbon phases is highly desirable. Therefore, in the present work buckypapers were produced from MWCNT suspensions and used as free-standing substrates to be coated with NCD by microwave plasma chemical vapour deposition (MPCVD). The integration of both allotropes was successfully achieved, the CNTs being preserved after diamond growth as confirmed by µ-Raman spectroscopy and SEM. Additionally, a good linkage was observed, the CNTs remaining embedded within the NCD matrix, thus reinforcing the interface of the resulting hybrid structure. This was corroborated by bending tests in a modified nano-hardness tester. The increase of the Young's Modulus from 0.3 to 300 GPa after NCD growth enables the use of this material in a wide range of applications including microelectromechanical systems (MEMS). Additionally, a highly anisotropic electrical resistivity behavior was confirmed: low in plane values were found for the CNT layer (1.39x10-2 Ω.cm), while high transverse ones were measured for both the NCD coated and uncoated CNT buckypapers (8.13x105 and 6.18x102 Ω.cm, respectively).