CaBi2Nb2O9-based (CBN-based) ferroelectric random access memory (FeRAM) has emerged as a promising candidate in the domain of data storage. Nevertheless, a comprehensive investigation into the enhancement of ferroelectric performance and the orientational configuration of FeRAM remains an area that has not been fully explored. Here, the CaBi2Nb2O9/SrRuO3/MgO (CBN/SRO/MgO) stack deposited at 750 °C shows a superior remanent polarization (Pr) of 18.43 μC/cm2 under only coercive field (Ec) of 192 kV/cm. The enhancement of ferroelectric properties can be attributed to the improved crystallinity and the increased random orientational distribution, particularly the deviation from the a-axis orientation. The grain size and grain orientation distribution of the material have been quantitatively analyzed using electron backscatter diffraction (EBSD). It has been revealed that specific orientations with higher Pop values are pivotal in enhancing the polarization switching. A TEM image indicates that a layer-by-layer structure is formed of the stacked films. These findings demonstrate a novel route to designing CBN-based ferroelectric memory devices tailored for information storage and data processing, showcasing the potential for integration into advanced smart electronics of the forthcoming era.