The construction and sub-molecular visualization of a self-organized adlayer of calix[4]arene on a Au(111) surface were achieved by potential-controlled adsorption and in situ STM. In situ STM images revealed that the self-organized molecular array consisted of a calix[4]arene dimer. The two molecules in a cone conformation with a sideways orientation were connected in a "head to head" orientation between the hydroxy groups.