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Abstract We report the pulsed‐laser deposition of epitaxial double‐perovskite Bi₂FeCrO₆(BFCO) films on the (001)‐, (110), and (111)‐oriented single‐crystal SrTiO₃substrates. All of the BFCO films with various orientations show theandsuperlattice‐diffraction peaks. The intensity ratios between the‐superlattice and the main 111‐diffraction peak can be tailored by simply adjusting the laser repetition rate and substrate temperature, reaching up to 4.4%. However, both optical absorption spectra and magnetic measurements evidence that the strong superlattice peaks are not correlated with theB‐site Fe³⁺/Cr³⁺cation ordering. Instead, the epitaxial (111)‐oriented Bi₂FeCrO₆films show an enhanced remanent polarization of 92 μC/cm²at 10 K, much larger than the predicted values by density‐functional theory calculations. Positive‐up‐negative‐down (PUND) measurements with a time interval of 10 μs further support these observations. Therefore, our experimental results reveal that the strong superlattice peaks may come fromA‐ orB‐site cation shifts along the pseudo‐cubic [111] direction, which further enhance the ferroelectric polarization of the BFCO thin films.