1-4 However, the significant drop in the dielectric constant with decreased film thickness, widely known as "size effect," has been reported to become serious. [1][2][3][4] The size effect in thin film dielectrics has made it difficult to design their performance characteristics. There has therefore been a strong motivation to discover size-effect-free highly insulating dielectric materials with a high dielectric constant. In this letter, we propose thin films with c-axis-oriented bismuth layer-structured dielectrics ͑BLDs͒ as candidates for size-effect-free materials.BLDs have a natural superlattice structure along the c axis consisting of two kinds of two-dimensional nanolayers, i.e., a bismuth oxide ͑Bi 2 O 2 ͒ 2+ sheet and a pseudoperovskite block generally described as ͑A m−1 B m O 3m+1 ͒ 2− , where m is the number of BO 6 octahedra in a pseudoperovskite block. Interestingly, BLDs with even m exhibit no ferroelectricity along the c axis. 5,6 In our previous study, we found that c-axis-oriented epitaxial SrBi 2 Ta 2 O 9 ͑SBT, m =2͒ films exhibited no degradation in dielectric constant down to 20 nm in thickness, corresponding to eight unit cells.7 However, their dielectric constant of 55 was obviously not enough to replace the conventional perovskite-structured oxides. We therefore expanded our concept to a higher m of 4, i.e., SrBi 4 Ti 4 O 15 ͑SBTi͒ and CaBi 4 Ti 4 O 15 ͑CBTi͒, to obtain higher dielectric constant and to deepen the understanding of the basic characteristics of c-axis-oriented BLD films. As a result, we found the design concept of their properties and revealed that thin films of c-axis-oriented BLDs are promising candidates for high-density capacitor application. c-axis-oriented epitaxial SBTi and CBTi films were grown at a substrate temperature of 700°C by metal organic chemical vapor deposition. ͑001͒ c -oriented epitaxial SrRuO 3 ͑SRO͒ films having an atomically flat surface grown on ͑001͒STO single crystals were used as substrates. 8 The constituent phase and the orientation were identified by conventional x-ray diffraction ͑XRD͒. The crystal structure was analyzed in detail by XRD using synchrotron radiation ͑SPring-8, BL13XU͒. 9 The dielectric and insulation properties of the films were measured after formation of the top electrodes of 100 m Pt on the film surface followed by postannealing in an electrical furnace at 400°C for 30 min under 1 atm flowing oxygen ambience.a͒ Electronic