We report detailed experimental results on the optical nutation effect in acetylene-filled hollow-core photonic crystal fibers (HC-PCFs). This coherent quantum optical effect is manifested by the appearance of attenuated oscillations in the profiles of transmitted step-like coherent optical pulses. The experiments used 15 ns optical pulses with peak powers up to ∼4 W and centered at 1530.37 nm, which corresponds to the acetylene (12C2H2) vibration-rotation resonance absorption line P9. The all-fiber cell made from a HC-PCF with internal diameter ∼10.3 μm contained a gas pressure of about 0.12 Torr. The Maxwell-Bloch equations are used to analyze the influence of the homogeneous relaxation, the inhomogeneous Doppler broadening of the absorption line, and the random orientation of the acetylene molecules. By comparing the experimental results with numerical simulations, we obtain the longitudinal and the transverse relaxation times to be close to 10 ns and find that the transition dipole moment of the acetylene P9 absorption line is ∼1.36×10−32 Cm.