structures of crystallites. [3][4][5][6] On a larger scale (i.e., >100 nm), ceramic crystal products are often hard and brittle, which was mainly affected by the structural dimensions and mesoscopic structures of the ceramic crystallites. [7][8][9] It has been reported that ceramic films were actually flexible when they were extremely thin (ex. several nanometers), and the flexibility was directly determined by the vibrations of chemical bonds. [10][11][12][13] Calculations have shown that the vibration energies of TiO, ZrO, and SiO bonds in inorganic crystals were much lower than those of CC, CO and CH bonds in organic polymers. [14] Generally, the high bonding density of ceramic crystals made ceramics hard, while crystal defects and amorphous oxides could produce soft mechanical responses. [15,16] Recently, several self-supporting oxide ceramic nanofibers (NFs) were fabricated by electrospinning. [17][18][19][20] Unfortunately, these NFs were not flexible, and they broke easily during stretching. Researchers tried to dop carbon or a second oxide phase into NFs to enhance the flexibility, but these NFs were still brittle due to the uncontrollable assembly of crystallites, which created randomly-arranged crystals with disorder grain boundaries and fine cracks. [21,22] Both of these structures were sensitive to rupture and rapidly aggregate into coarse cracks when NFs were subjected to external forces. [23][24][25] Here, we define "flexible" electrospun NFs as those in which the individual NF is compliant (small elastic modulus) and strong (high yield strength), as opposed to stiff and weak. Once these flexible NFs stagger randomly together to form membranes, they can undergo large deformation without fracture and thus demonstrate silk-like softness property. However, the membrane thickness should be considered when reporting the flexibility of such ceramic NF membranes.Here, we explore how the mesoscopic structure of such crystallites can be designed to create flexible electrospun ceramic NFs and propose a reasonable expression of ceramic flexibility when considering the influence of thickness. Inspired by the "Magic Ruler Puzzle" that is generally composed of a rigid triangular prism (brick) and soft spring (mortar) in an ordered arrangement, we fabricated superior flexible TiO 2 NFs with similar brick-and-mortar structures by combining ball-milling and curved-drafting strategies with traditional sol-gel electrospinning. This method produced flexible TiO 2 NF membranes that could fold without tearing, and the individual NF Oxide crystal ceramics are commonly hard and brittle, when they are bent they typically fracture. Such mechanical response limits the use of these materials in emerging fields like wearable electronics. Here, a polymerinduced assembly strategy is reported to construct orderly assembled TiO 2 crystals into continuous nanofibers that are stretchable, bendable, and even knottable. Ball-milling the spinning sol and curved-drafting the electrospun nanofibers significantly improve the molecula...