To improve the data accuracy of the neutron emission spectra of the natLi(d,xn) reaction that will be used as the neutron source in the International Fusion Materials Irradiation Facility, the authors have measured the neutron emission spectra from thick and thin lithium targets bombarded by 40-MeV deuterons at the AVF cyclotron (K = 110) facility of Tohoku University. The neutron spectra were measured at nine laboratory angles between 0 and 110 deg with the time-of-flight method using a beam-swinger system and a well-collimated neutron flight channel, obtained over almost the entire energy range of secondary neutrons using a two-gain method. The data obtained revealed the shape and angular dependence of emission spectra up to the high-energy region called a "high-energy tail." The experimental results are compared with other experimental data and calculations.