Integral neutronics experiments have been the powerful tool and method for examining the reliability of the evaluated nuclear data. In present paper, the accuracy of evaluated nuclear data for zirconium has been validated by comparing measured leakage neutron spectra with calculated ones. Leakage neutron spectra from the irradiation of D-T neutrons on zirconium samples were experimentally measured at 60° and 120° by using a time-of-flight method. Theoretical calculations are carried out by the Monte Carlo neutron transport code MCNP-4C with the evaluated nuclear data of the ENDF/B-VII.0, ENDF/B-VIII.0, JENDL-4.0 and CENDL-3.1 libraries. From the comparisons, it is found that the calculations with JENDL-4.0 gives better agreements with the experiments at 60° while a large discrepancies are observed in the 4–13.5 MeV energy range at 120°. However, the calculated spectra using the data from ENDF/B-VII.0, ENDF/B-VIII.0 and CENDL-3.1 libraries showed some discrepancies with the measured ones, especially caused by the difference of the elastic and inelastic angular distributions and the secondary neutron energy distributions in the continuum inelastic scattering.