Well-ordered large-area arrays of ferroelectric La-substituted Bi4Ti3O12 (BLT) nanostructures were prepared by pulsed laser deposition using gold nanotube membranes as shadow masks. By x-ray diffraction and transmission electron microscopy, it was found that well-defined (001)-, (118)/(100)-, and (104)-oriented BLT nanostructures were obtained on (001)-, (011)-, and (111)-oriented SrTiO3 single crystal substrates covered with epitaxial SrRuO3 electrode layers, respectively, through ex situ crystallization at 700 °C. Atomic force microscopy analyses revealed that the epitaxial BLT nanostructures maintain a height of about 100 nm and a lateral size of about 150 nm in spite of the postannealing process. The anisotropic ferroelectric properties of the BLT nanostructures of three different orientations were investigated by scanning force microscopy in piezoresponse mode. The highest effective remanent piezoresponse coefficient (2dzz) of about 38.0 pm/V was observed in (118)/(100)-oriented BLT nanostructures, whereas (001)- and (104)-oriented nanostructures showed smaller 2dzz values of 5.0 pm/V and 1.4 pm/V, respectively.