The authors’ results on synthesis of catalytic filamentous carbon (CFC) on supported Ni- and Co-catalysts via pyrolysis of C₃-C₄ alkanes were summarized. The supported catalysts were prepared by homogeneous precipitation of metal hydroxides nanoparticles on starting inorganic carriers that were varied in chemical origin (Al/Si, silica, Al₂O₃, carbon) as well as in texture and macrostructure (honeycomb monolith, foams, rods, rings). The conditions of preparation of catalysts as well as C₃-C₄ pyrolysis were selected in order to synthesize carbon nanofilaments of 50-100 nm in diameter and 1-2 µ. A thin surface layer of catalytic filamentous carbon (CFC-layer) was formed via chaotically interlacing these nanofilaments and coated uniformly the macroporous and macrostructured starting carriers. The morphology of the precipitated metal hydroxide nanoparticles and synthesized carbon deposits, in particular carbon nanofilaments were examined by scanning electron microscopy. Nanoparticles of Ni or Co hydroxides of the size 200-500 nm were found to exhibit the highest catalytic activity and ensure the maximal carbon yield (~40-80 g of CFC/g of supported Me) in the one-stage C₃-C₄ pyrolysis in the presence of hydrogen (H₂). The texture parameters of CFC-layered adsorbents were determined by physicochemical methods. Mesopores of 10-50 nm in diameter were found to be predominant in CFC-layer; and specific surface area increased by an order of magnitude from 0.5-1 m²/g of the macroporous/macrostructured starting carriers up to 10-60 m²/g of the final adsorbent. These composite CFC-layered adsorbents were applied in heterogeneous biocatalysis for immobilization of the enzymatic active substances. The properties (activity and stability) of heterogeneous biocatalysts were studied. As an example, CFC-layered Ni/graphite rods were tested as anodes for microbial fuel cell. The bacterial cells of Gluconobacter oxydans were adhered on such anodes, and the electrochemical parameters of designed microbial fuel cell were determined; and power density of ~25 mW/m² was achieved.