Encoding information in light polarization is of great importance in facilitating optical data storage (ODS) for information security and data storage capacity escalation. However, despite recent advances in nanophotonic techniques vastly enhancing the feasibility of applying polarization channels, the data fidelity in reconstructed bits has been constrained by severe crosstalks occurring between varied polarization angles during data recording and reading process, which gravely hindered the utilization of this technique in practice. In this paper, we demonstrate an ultra-low crosstalk polarization-encoding multilayer ODS technique for high-fidelity data recording and retrieving by utilizing a nanofibre-based nanocomposite film involving highly aligned gold nanorods (GNRs). With parallelizing the gold nanorods in the recording medium, the information carrier configuration minimizes miswriting and misreading possibilities for information input and output, respectively, compared with its randomly self-assembled counterparts. The enhanced data accuracy has significantly improved the bit recall fidelity that is quantified by a correlation coefficient higher than 0.99. It is anticipated that the demonstrated technique can facilitate the development of multiplexing ODS for a greener future.