Improvement of carbon-based buildings composed of nanoparticles with totally different kind of orbital hybridization of carbon (sp2, sp3) made it doable to create new substances with superior biomedical properties, luminescent, and magnetic when the carbon parts are modified by lanthanides for the purposes in Photodynamic Remedy or Magneto-Resonance Imaging. The offered outcomes are dedicated to the synthesis, physical-chemical and synchrotron research of water-soluble complexes of detonation nanodiamonds (particle dimension 4–5 nm) and fullerenols Gd@C82(OH)X (X ∼ 30). The affiliation of positively charged diamonds and electro-negative fullerenols created the complexes being steady below heating (25–70 °C) whereas the meeting of fullerenols with the diamonds carrying unfavourable floor expenses was much less possible. Small angle scattering of synchrotron radiation revealed the affiliation of diamonds into chain-like buildings extra steady attributable to further linking of diamonds through fullerenols. On account of complexing, fullerenols received magnetic resonance properties of unfavourable contrasting substances for MRI diagnostics. The exams on organic cells confirmed a low toxicity of complexes which can be utilized as potential biomedical supplies.