We report the use of terahertz time-domain spectroscopy (THz-TDS) to probe chiral self-assembled twisted nanoribbons from a ferrocene-modified dipeptide consisting of two (L)-amino acids (Fc-FF). Supported by molecular dynamics simulation, the THz absorption peaks at 0.9 THz and 2.7 THz are attributed to distinct characteristic vibrational modes of Fc-FF single crystal. The relative absorption intensity is introduced to characterize the discrepancy in THz peak absorption which originates from symmetry breaking. Combined with the results of scanning electron microscopy, circular dichroism, Fourier transform infrared spectroscopy and X-ray diffraction, THz-TDS unravels great potentials to distinguish subtle structural changes within chiral self-assembled materials.