We report observation of holographic surface relief gratings with relatively large amplitude on a second order nonlinear optical polymeric material. Surface relief gratings on these polymer films were created upon exposure to polarized Ar+ laser beams at 488 nm without any subsequent processing steps. The surface structure of the relief gratings was investigated by atomic force microscopy. The depth of the surface relief in a typical case was 120 nm which is approximately 20% of the original film thickness. The diffraction efficiency of gold‐coated gratings was investigated as a function of wavelength and capability of recording orthogonal gratings on the same film was demonstrated.