Sputter deposited CoCr(Mo)/Si film were studied with emphasis on the correlation between magnetic properties and crystallographic orientation. The perpendicular coercivities of CoCr films decreased with Si underlayer thickness, whereas those of CoCrMo films increased with Si underlayer thickness. It has been explained that additions of the larger atomic radius Mo atoms in CoCr films impedes crystal growth resulting in a decrease in grain size, thus this small grain size may induce high perpendicular coercivity. The c-axis alignment of CoCrMo film was improved due to addition of 2at.%Mo. It means CoCrMo layer grow self-epitaxial directly from orientation and structure of Si underlayer when the main layer grow on underlayer.