The aim of the present work is to shed some light on the surface atomic structure of an Fe/Mn-promoted sulfated zirconia catalyst using high-resolution transmission electron microscopy (HRTEM) imaging. The presence of Fe and Mn species, which were found to be dispersed at a molecular level, were apparent on the {001} and {110} surfaces of zirconia particles. A combination of the present results with additional detailed studies using other physicochemical characterization techniques is needed to elucidate the atomic configuration of the active sites responsible for the enhanced catalytic activity of the Fe/Mn-promoted sulfated zirconia catalyst.