Experimental cross section data of the 67 Zn(n,α) 64 Ni reaction are very scanty because the residual nucleus 64 Ni is stable and the commonly used activation method is not feasible. As a result, very large deviations (about 10 times) exist among different nuclear data libraries. In the present work, cross sections of the partial 67 Zn(n,α 0 ) 64 Ni and total 67 Zn(n,α) 64 Ni reactions are measured at neutron energies of 4.0 and 5.0 MeV for the first time, and those of 6.0 MeV are remeasured for consistency checking. A twin-gridded ionization chamber was used as the charged-particle detector and two enriched back-to-back-set 67 Zn samples were adopted. Experiments were performed at the 4.5 MV Van de Graaff Accelerator of Peking University. Neutrons were produced through the 2 H(d, n) 3 He reaction using a deuterium gas target. Absolute neutron flux was determined by counting the fission fragments from a 238 U sample placed inside the gridded ionization chamber while a BF 3 long counter was employed as neutron flux monitor. Present data are compared with results of previous measurements, evaluations, and TALYS code calculations.