LAUSR

Programmable base pair interactions at the nanoscale make DNA an attractive scaffold for forming hydroxyapatite (HAP) nanostructures. However, engineering macroscale HAP mineralization guided by DNA molecules remains challenging. To overcome this issue, a facile strategy is developed for the fabrication of ultrastiff DNA–HAP bulk composites. The electrostatic complexation of DNA and a surfactant with a quaternary ammonium salt group enables the formation of long‐range ordered scaffolds using electrospinning. The growth of 1D and 2D HAP minerals is thus realized by this DNA template at a macroscale. Remarkably, the as‐prepared DNA–HAP composites exhibit an ultrahigh Young's modulus of ≈25 GPa, which is comparable to natural HAP and superior to most artificial mineralized composites. Furthermore, a new type of dental inlay with outstanding antibacterial properties is developed using the stiff DNA–HAP. The encapsulated quaternary ammonium group within the dense HAP endows the composite with long‐lasting and local antibacterial activity. Therefore, this new type of super‐stiff biomaterial holds great potential for oral prosthetic applications.