To verify the performance of the neutron total cross-sectional spectrometer, the neutron total cross section of carbon is initially measured in the energy range of 1 eV to 20 MeV using the time-of-flight method. The measure-ment is performed at the Back-n white neutron source with a 76-m time-of-flight path using the China Spallation Neutron Source. A multilayer fast fission chamber with 235U and 238U is employed as the neutron detector. The diameter and thickness of the natural graphite sample are 70 mm and 40 mm, respectively. Signal waveforms are collected using a data acquisition system. Off-line data processing was used to obtain the neutron time-of-flight spectra and transmissions. The uncertainty of the counting statistics is generally approximately 3% for each bin in the energy range of 1–20 MeV. It is determined that the results for the neutron total cross section of carbon obtained using 235U cells are in good agreement with the results obtained using 238U cells within limits of statistical uncertainty. Moreover, the measured total cross sections show good agreement with the broadening evaluated data.