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This contribution reports for the first time on the synthesis and the main physical properties of single-phase pure α-Cr2O3 nanoparticles synthesized by a facile, rapid and eco-friendly process using Callistemon viminalis flower's extract as an effective oxidizing/reducing agent. These crystalline nanoparticles exhibit a cubic-like platelet shape with sharp edges with an average particle diagonal size of ∼92.2 nm. The room temperature physical properties of these pure highly crystalline Eskolaite α-Cr2O3 nanoparticles were carried out using complementary techniques such as high-resolution transmission electron microscopy (HRTEM), energy-dispersive X-ray spectroscopy (EDS), XRD, FTIR-ATR, Raman and XPS.