New type of carbon based nanostructure on the vicinal 3C-SiC(111)-4° and 3CSiC(111)-8° surfaces with adsorbed Ba and Cs nanolayers has been found. The 3C-SiC(111)- 4° (8°) samples were grown by low-defect unstressed nanoscaled films epitaxy method on silicon vicinal substrates. Electronic structure of the 3C-SiC(111)-4° (8°) surfaces and the (Ba, Cs)/3C-SiC(111)-4° (8°) interfaces has been detailed studied in situ in an ultrahigh vacuum by synchrotron-based photoelectron spectroscopy. The C 1s, Si 2p, Ba 4d core levels and valence band spectra were investigated as a function of Ba or Cs submonolayer coverages. A special fine structure of the C 1s core level spectrum was revealed to appear under Ba and Cs adsorption on the vicinal SiC surface only. Drastic change in the C 1s spectrum was ascertained and shown to be originated from the interacting Si vacancy and adsorbed Ba (Cs) atoms initiating both the electron redistribution and surface reconstruction effects with formation of a new type of the C-enriched graphitic-like nanostructure.