A new synthetic route was applied to develop carbon nanofiber (CNF)-layered double hydroxide (LDH) hybrid through a noncovalent assembly using sodium dodecyl sulfate as bridging linker between magnesium-aluminum LDH and CNF and then characterized. Furthermore, this hybrid was used as nanofiller in thermoplastic polyurethane-acrylonitrile butadiene rubber (TN; 1:1 w/ w) blend. Mechanical measurements showed that the 0.50 wt % hybrid loaded TN blend exhibited the maximum improvements in the elongation at break, tensile strength, and storage modulus of 1.51 times and 167 and 261% (25 8C), respectively. Differential scanning calorimetric analysis and thermogravimetric analysis showed maximum improvements in the melting temperature (5 8C), crystallization temperature (17 8C), and thermal stability (14 8C) in the 0.50 wt % surfactant modified carbon nanofiber-LDH loaded blend compared to the neat blend. Such enhancement in the properties of the TN nanocomposites could be attributed to the homogeneous dispersion, strong filler-blend interfacial interaction, and synergistic effect.Polymer blends are prepared by a combination of at least two polymers with properties that are different from their individual components. 11,13,25,26 They can be divided into immiscible, miscible, and compatible polymer blends. However, considerable attention has been focused on compatible polymer blends because of the attainment of balanced properties. 13,25 Furthermore, these polymer blends, having a variety of nanofillers, are Additional Supporting Information may be found in the online version of this article.