The first four members of Bi-layered Srm-3Bi4TimO3m+3 homologous series with m=3, 4, 5, and 6, i.e., Bi4Ti3O12, SrBi4Ti4O15, Sr2Bi4Ti5O18, and Sr3Bi4Ti6O21, were grown on SrTiO3 (001) single-crystal substrates by pulsed-laser deposition. X-ray diffraction and high-resolution transmission electron microscopy (HRTEM) reveal that the films grew epitaxially with in-plane epitaxial alignment of [11¯0]Srm-3Bi4TimO3m+3∥SrTiO3. HRTEM cross-sectional images show that the films with m=3, 4, and 5 are nearly free of intergrowth, whereas a number of growth defects were observed in the film with m=6. Using an evanescent microwave probe, the room-temperature dielectric constants of these epitaxial films are measured to be 221±13, 205±15, 261±29, and 249±17 for films with m=3, 4, 5, and 6, respectively. © 2002 American Institute of Physics.