This work was supported by a Grant-in-Aid for Young Scientists (B) (No. 21750155) and for Scientific Research in a Priority Area “Super-Hierarchical Structures” (No. 19022036) from the MEXT and Ritsumeikan R-GIRO project (2008–2013). The authors thank Prof. Atsuhiro Osuka, Dr. Shohei Saito, and Eiji Tsurumaki, Kyoto University, for single-crystal X-ray analysis, Dr. Takashi Nakanishi, National Institute for Materials Science, for SEM measurements, Prof. Kazuchika Ohta and Shohei Shimosugi, Shinshu University, for preliminary examinations on charge-by-charge assemblies, Prof. Tomonori Hanasaki and Shunichi Murayama, Ritsumeikan University, for DSC measurements, SPring-8 (JASRI) for synchrotron radiation experiments at BL40B2 (No. 2009A1985, 2009B1593, 2010A1504, and 2010A1621), and Prof. Hitoshi Tamiaki, Ritsumeikan University, for various measurements. Y.H. thanks JSPS for a Research Fellowship for Young Scientists.