Conformational dynamics of biomolecules, which can span very large time scales ranging from seconds down to femtoseconds, play a key role in their function. In this regard, the combination of the high temporal resolution of ultrafast pump–probe spectroscopy and the structural sensitivity of electronic circular dichroism (CD) spectroscopy provides an extremely promising tool to follow these dynamics with a "virtually" unlimited temporal resolution. However, although CD spectroscopy is a widely used tool in structural biology to determine the secondary structure of biomolecules in solution, transposition of these measurements to the time domain (TRCD), on the sub-picosecond time scale, remains very challenging due to their weak signals prone to pump-induced polarization artifacts. Recent advances in laser technologies and non-linear optics, however, offer new perspectives for the development of femtosecond TRCD set-ups. In this review, we present recent developments in ultrafast TRCD spectroscopy. We discuss the advantages and drawbacks of the few existing functional experimental set-ups for their use to access the conformational dynamics of biomolecules at ultrashort time scales.