In the present work, a controlled production of carbon nanospheres (CNS) via pyrolysis of benzene, aniline and nitrobenzene at 950 °C has been examined. The nature of the carbonaceous product has been characterized by transmission electron microscopy (TEM), N2 adsorption/desorption, X-ray diffraction (XRD), elemental analysis (CHN), temperature-programmed oxidation (TPO) and X-ray photoelectron spectroscopy (XPS). Time-on-stream served to enhance the spherical morphology of the product, as well as its crystalline character. Nitrogen inclusion resulted in an enhanced curvature of the graphene layers, as well as the incorporation of lattice defects, resulting in a less crystalline material. The reactive nature of the feed influenced the amount of nitrogen incorporated into the carbon matrix, as well as the kind and distribution of nitrogen functionalities. © 2009 Elsevier B.V. All rights reserved.