Super-large-period Aurivillius thin films with a pseudo-period of ten were grown on (0 0 1) SrTiO 3 substrates using the pulsed laser deposition method. The as-grown films are found to be coherently strained to the substrate and atomically smooth. X-ray diffraction indicates an average periodicity of ten, while analysis with the high resolution scanning transmission electron microscopy reveals a self-modulated nanostructure in which the periodicity changes as the film thickness increases. Finally, we discuss the magnetic and possible ferroelectric properties of the self-modulated large period Aurivillius films at the room temperature. V C 2015 AIP Publishing LLC.[http://dx.doi.org/10.1063/1.4921966] Double-magnetic-ion doped Aurivillius phase oxides, 1-3 potentially as the single-phase candidate that could exhibit both ferroelectricity (FE) and ferromagnetism (FM) above the room temperature, have recently attracted intensive attentions in the multiferroic community. The general formula of the Aurivillius oxides can be simply as (Bi 2 O 2 ) (A mÀ1 M m O 3mþ1 ), where A ¼ Bi 2þ , Ba 2þ , Ca 2þ , Sr 2þ , etc., and M ¼ Fe 3þ , Co 3þ , Ni 3þ , Ti 4þ , Ta 5þ , Nb 5þ , etc. 4,5 The lattice structure could be regarded as with the pseudo perovskite slabs (A mÀ1 M m O 3mþ1 ) 2À inserted into the fluorite-like bismuth-oxygen bilayers. However, synthesis of such large period structures can be obviously challenging due to the structural instability. Yet understanding such materials would be important for finding new multiferroic material. 6-8 Recently, large period Aurivillius phases have been mostly studied in the bulk ceramic format. 9-12 Unfortunately, bulk ceramic synthesis is usually with the secondary phase generation, 2,13,14 which can become more severe for complex structures with large period number of m. Adopting of single crystalline thin film for the studies would be more favorable, yet a successful growth of such films is very challenging.Hetero-epitaxial growth is privileged in realizing artificial structures that are unstable in their bulk formats, 15 and this may be true for the Aurivillius structures with large periodicity. In non-magnetic Aurivillius Sr mÀ3 Bi 4 Ti m O 3mþ3 (SBTi) system, 16-20 period as large as m ¼ 8 has been realized by the thin film epitaxy. 21 Very few work has been reported about the epitaxial fabrication of thin films with periods larger than 8. Therefore, it would be interesting to explore the growth limit on the period, together with the pressing demand for multiferroic Aurivillius phase thin films with very large period numbers. Among different combinations of double-magnetic ion (Fe-Co, Fe-Mn, Fe-Ni, etc.) doped multiferroic Aurivillius ceramics, Fe-Co doped Bi mþ1 (Fe,Co) mÀ3 Ti 3 O 3mþ3 (BFCTO, m ¼ 4) has been reported with relatively strong FM and FE orders above the room temperature. 3,22 The FM order becomes stronger in larger periods m ¼ 5 and 6 BFCTO systems. [23][24][25][26] It is important to study the fundamental growth mechanism in the epitaxial synthesis of large perio...