In this study, for developing microsensors for weak magnetic field, methods for developing high permeability nanocrystalline permalloy by electrodeposition and the relationship between the grain size and magnetic properties of the nanocrystalline permalloy are investigated. By dc plating with and without saccharin added and pulse plating with saccharin added, permalloy samples of grain sizes from 52 nm to 11 nm are obtained. The coercivity and magnetoimpedance (MI) ratio of the samples are tested against the grain size variation. Results show that the coercivity decreases rapidly and MI ratio increases greatly with grain size decrease from 52 nm to 11 nm. (c) 2005 American Institute of Physics.