In recent years, flexible functional materials have attracted increasing interest, but there is a lack of designing mechanisms of flexibility design with superstructures. In traditional engineering mechanics, the maximum bending strain (MBS) was considered universal for describing the bendable properties of a given material, leading to the universal designing method of lowering the dimension such as thin membranes designed flexible functional materials. In this work, the MBS was found only applicable for materials with uniformly distributed Poisson's ratio, while the MBS increases with the thickness of the given material in case there is a variation Poisson's ratio in different areas. This means the MBS can be enhanced by certain Poisson's ratio design in the future to achieve better flexibility of thick materials. Here, the macroscopic freestanding inorganic functional BaTiO3:Sm3+ (BTO:S) nanofiber membranes, which have a nonconstant Poisson's ratio response on stress/strain for creating nonuniformly distributed Poisson's ratio, were proven applicable for designing larger MBS and lower Young's modulus for flexible functional materials.