Inclusion of Ti, Mn and Fe cations (necessary to achieve the m = 5 multiferroic phase), results in a complex bonding environment for the transition metal cations at the perovskite-type B-sites of the B6TFMO Aurivillius phase structure (Figure ). Previous electron microscopy and density functional theory (DFT) descriptions of the atomic structure, along with demonstration of the preferred magnetic cation locations (see Supporting Information (SI) section 1), has progressed our understanding of the fundamental mechanisms governing ferromagnetism in this interesting single phase multiferroic. However, it is recognized that functional electric and magnetic properties that drive application in information storage are strongly correlated with octahedral tilting and local structural distortions within perovskite systems and their heterostructures , , , , . Therefore, tailoring of the B6TFMO composition to enhance multiferroic behavior needs a detailed understanding of atomic-level influences of local symmetry lowering distortions and octahedral tilting on the fundamental electronic structure, ferroelectric properties and magnetic coupling interactions that arise from differing chemical bonding environments. This knowledge is currently lacking for B6TFMO multiferroics.