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Carbon nanoflakes (CNFs) are a promising carbon nanomaterial that can be used as a catalyst, an adsorbent, or as a matrix for stabilization of oxide nanoparticles, including Ln2O3 used as contrast agents for computed tomography [1]. CNF particles transform into onion-like carbon (OLC) particles under spark plasma sintering (SPS) treatment [2]. The present work is devoted to the synthesis of OLC particles, their heterosubstituted analogies, and core-shell structures Ln2O3@C produced via SPS of CNFs, N-, P-, Si-CNFs and Ln2O3 deposited on the CNF surface.