We have studied the surface morphologies and magnetic properties of Fe and Co thin films evaporated on polyethylene naphthalate (PEN) organic substrates toward the fabrication of spin quantum cross devices. As a result, the surface roughnesses of Co (6.1 nm)/PEN and Co (12 nm)/PEN are as small as 0.1 and 0.09 nm, respectively, corresponding to less than one atomic layer, in the same scanning scale as the thickness. As for the magnetic properties, the coercive force of the Co/PEN shows the constant value of 2 kA/m upon decreasing the Co thickness from 35 to 10 nm, and it increases up to 7 kA/m upon decreasing the Co thickness from 10 to 5 nm. It decreases when the Co thickness is less than 5 nm. These results can be explained by the competition between the shape magnetic anisotropy and the induced magnetic anisotropy