The chemistry of carbon dots (CDs) surface has enabled the development of new luminescent nanomaterials with wide and precise array of applications. In respect to this, we perform the surface passivation of carboxylated carbon nanoparticles with the aromatic 1,2-phenylenediamine to prepare water-soluble photoluminescent CDs exhibiting a photoluminescence (PL) quantum yield of 8% at 575 nm, a composite photoluminescence signal in the 330-500 nm domain, and an average lifetime of 1.93 ns. This new synthetic strategy promoted the formation of carbon dots covered with benzimidazole-containing oligomers of 1,2-phenylenediamine (o-PD) that, by taking advantage of the benzimidazole derivatives' biological activity and their application in Material Science, could lead to various new applications.