In the case of sp2 amorphous carbons, formed by nanoscale graphene domains framed by heteroatom necklaces (basic structure units in total), inelastic neutron scattering and photoabsorption ensure studying vibrational spectra of the latter mainly. Examination of a set of samples of the highest carbonization rank representing natural substances (shungite carbon, anthraxolite, and anthracite), technical graphenes (laboratory reduced graphene oxides), and industrial products (carbon blacks) has shown, that while INS spectra revealed the hydrogen-enriched component of these necklaces only, the DRIFT spectra exhibited two components determined by both hydrogen and oxygen compositions. Taking together, INS and DRIFT spectra exhibit methine groups, typifying the hydrogen component of all natural amorphics as well as hydroxymethyls and methyls doing the same job for the studied technical graphenes, and hydroxyfurans - for carbon blacks. A comparable analysis of DRIFT and XPS spectra has allowed a reliable personification of the oxygen functional groups compositions. Based on the results obtained, a set of reliable molecular models of the amorphics’ basic structural units has been proposed. © 2020 Taylor & Francis Group, LLC.