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Multi-walled carbon nanotubes (MWCNTs) are widely recognized for their exceptional mechanical properties and potential to reinforce composite materials. However, the requirement for high MWCNT concentration remains a challenge in achieving effective reinforcement. In this study, using unzipped multi-walled carbon nanotubes (uMWCNTs) and transition metal filler as a means to significantly enhance the mechanical properties of polyamide 66 (PA66) and incorporating 0.2% w/w of uMWCNTs-Mn as filler allowed us to increase PA66's tensile strength by over 74% and its Young's modulus by over 100%. The structural and functional integrity of uMWCNTs-Mn and PA66 matrix were investigated in detail. This work reveals that the enhancement of mechanical properties is mainly due to the interfacial interaction between uMWCNTs-Mn sheets and the PA66 matrix, the coupling effect of manganese ions, and increases the crystallinity and reduces the size of microcrystals. This work's findings provide a novel approach to the preparation of high-performance composites with low concentrations of carbon nanostructures, which holds significant implications for the development of advanced materials.