A manufacturing method of an electron-emitting device including the steps of: preparing a base substrate provided with an insulating or semi-conducting layer in advance and exposing the layer to an atmosphere which contains neutral radical containing hydrogen. It is preferable that the insulating or semi-conducting layer contains metal particles; the insulating or semi-conducting layer is a film containing carbon as a main component; the neutral radical containing hydrogen contains any of H., CH3., C2H5., and C2H. or mixture gas thereof; compared with a density of a charged particle in the atmosphere, a density of the neutral radical containing hydrogen in the atmosphere is more than 1,000 times; and a step of exposing the insulating or semi-conducting layer to the atmosphere is a step of making a hydrogen termination by using a plasma apparatus provided with a bias grid.