Heteroepitaxial growth of copper phthalocyanine (CuPc) on Au(111) surfaces has been confirmed for the first time by Scanning Tunneling Microscopy (STM). The combination of in situ electron diffraction (RHEED) with STM allows direct studies of heterogeneous layer growth, revealing a novel commensurable superstructure of the organic overlayer with the Au(111) surface. The organic molecular beam epitaxy (OMBE) technique has demonstrated that molecular orderings of CuPc monolayers can be controlled, resulting in artificial lattice structures in organic ultrathin films being different from those in bulk.