We herein report the controllable synthesis of spherical cobalt ferrite nanoparticles with average crystallite size in the range of 3.6–12.9 nm using a facile, eco-friendly, hydrothermal method. The hydrothermal treatment was carried out by utilizing cobalt nitrate, ferric nitrate, and ammonium hydroxide in the presence and absence of Arabic gum as a surfactant agent. The purity and crystallinity of the products were tuned by varying reaction conditions such as reaction time (0.5–8 h), reaction temperature (120– 180
C), percentage of ethylene glycol (0–100% (v/v)), pH (8–9.6), and amount of Arabic gum (0–2 g). We characterized the prepared products using X-ray diffraction (XRD), field-emission scanning electron microscopy (FE-SEM), Fourier transform infrared spectroscopy (FT-IR), high-resolution transmission electron microscopy (HR-TEM), energy-dispersive X-ray spectroscopy analysis (EDS), selected area electron diffraction (SAED) patterns, and UV-visible diffuse reflectance spectra (DRS). The optimal hydrothermal treatment was performed at 180
C and pH 9.6 for 4 h in aqueous media. The results also revealed that the as-prepared spinel cobalt ferrite nanoparticles have an estimated optical band gap energy in the range of ca. 1.6–1.9 eV, indicating the semiconducting characteristics of the products.