Naturally short-length multi-walled Russian-doll-like carbon nanotubes derived by a catalyst-free arc-discharge method were used as nano-sized “cutters” to transform bulk graphitic sheets into thin/few-layered graphene-like nano-sized platelets (GNPs) during a jet milling procedure. A short follow-up oxygen plasma treatment in a plasma reactor further increases the number of smaller (i.e. ∼80 nm) and thinner nanoparticles (i.e. three-layered GNPs) as well as their oxygen content (i.e. up to ∼8 at.%). These oxygen-rich surface-functionalized GNPs are suitable additives for producing stable nanogels as demonstrated by the preparation of carbon ink dispersions.