The nanocrystalline Ni films were grown on n-Si(111) substrate by Pulsed electrodeposition in non-aqueous NiCl(2) + methanol solution. The frequency of potential pulse was modulated during the deposition of Ni onto Si substrates. When the frequency varies from 20 to 900 Hz, the average size of Ni nanocrystallites varied in the ranges from 48 to 130 nm. In these cases, all Ni films have grown through a three-dimensional instantaneous nucleation followed by diffusion-limited growth. From X-ray diffraction measurement, it has been found that Ni(111) grows preferentially on the Si(111) substrates. The magnetic hysteresis loops for as-deposited films were measured by using VSM. As the angle 0 between film plane and applied magnetic field varies from 0 to 90, the coercivity (H(c)) and squareness (S) obtained from the magnetic hysteresis loops showed an opposite behavior. With the increase in 0, H(c) increased but S decreased near linearly. We have also investigated the variation of H(c) as a function of Ni nanocrystallite's size. From VSM measurement, we could observe that the coercivities for the magnetic field applied perpendicular and parallel to the film plane increase up to the average size of 86 not but begin to decrease over this size. (C) 2009 Elsevier B.V. All rights reserved.