The surface structure of polycrystalline Fe films of various thicknesses on glass substrates have been studied using a Ti: Sapphire laser at 780 nm. We found that the surface structure possesses Cs crystal structure close to
C2v through symmetry consideration. We present one-fold intensity profile with one mirror plane in second harmonic (SH) intensity as a proof of Cs symmetry. Cs and C2v surface symmetries usually appear at the (110)
surface of a cubic diamond single crystal [1]. Therefore this surface symmetry would be related to bcc (110) growth orientation coinciding with XRD measurement. Further we treated surface normalized SH asymmetry
with various thicknesses. The SH asymmetry increases with increasing of film thickness. From these results, it is observed that the surface structure of thin polycrystalline Fe film below 5 nm is almost isotropic, while in the case of the thicker Fe films, surface structure have Cs symmetry structure close to C2v.