Despite many studies of nanomaterials have been reported on the enhancement of cement-based materials, such as the pozzolanic effect of nano silica and flexural enhancement of fibers, there rarely are reports of the nanomaterials with both pozzolanic effect and shape-based enhancement. In this paper, anisotropic nanofibers were synthesized based on calcium silicates through hydrothermal method. Seed-mediated growth was conducted while SiO2 nanoparticles served as the seeds and pseudo-wollastonite was used as the precursor. Importantly, the addition of the nanofibers can greatly improve the 28d flexural strength from 7.12 MPa to 8.99 MPa of the cement-based materials, which provides a new approach to realize the high performance of cement-based materials.