Abstract: The bond performance between fibers and the matrix in fiber-reinforced cement-based composites has a significant impact on their macroscopic mechanical properties. Twisted steel fibers, due to their unique surface characteristics, have the potential to enhance fiber-matrix bonding. To investigate the bonding performance of twisted steel fibers in polyvinyl alcohol fiber-reinforced cement-based composites (PVA-ECC), single fiber pull-out tests were conducted on 30 designed dog-bone-shaped specimens, considering factors such as fiber type, steel fiber aspect ratio, matrix water-binder ratio, and PVA fiber content. The results indicate that the bond strength of twisted steel fibers in the matrix is 2.06 times and 4.80 times that of hooked-end and straight steel fibers under the same conditions, respectively. Increasing the diameter of twisted steel fibers, reducing the matrix water-binder ratio, and increasing the PVA fiber content (up to 2%) significantly improve the bonding performance of twisted steel fibers in the matrix. Additionally, macroscopic mechanical performance tests on the hybrid twisted steel fiber/PVA-ECC demonstrate the superior strength and toughness of this novel fiber-reinforced cement-based composite.