AbstractDynamic toroidal dipole (TD) with its peculiar characteristic of broken space‐inversion and time‐reversal symmetries plays an important role in the fundamental physics of light–matter interaction. Here, TD metamaterials comprised of amorphous silicon nanopillar arrays embedded in spin‐on‐glass layer are experimentally demonstrated. Upon normal incidence of plane wave, the transverse toroidal moment and the associated anapole‐like state are excited in optical regime. The strong TD response stems from a complete head‐to‐tail configuration of the magnetic dipole moments within each individual nanopillar. Both the experimental and simulation results show that such TD mode sustains a large structural tolerance and can be spectrally tuned by elongating the cylindrical axis perpendicular to the light polarization, corresponding to a cross‐sectional variation from circular to elliptical shapes. The excited TD mode is found to exhibit ultrahigh refractive index sensitivity compared to other multipoles, resulting in a sensitivity of 459 nm (470 nm) per external refractive index change in the experiment (calculation). This approach provides a simple and straightforward path in realizing toroidal metamaterials and establishes a new flat‐optics platform for realizing active metadevices, sensors, and nonlinear nanophotonics.