A series of layered double hydroxides interleaved with surfactant using saturated alkyl chain carboxylate anions CH3(CH2)mCOOH, even number m between 6 (C8) and 16 (C18), obtained by coprecipitation method was dispersed by melt polymer extrusion into polypropylene (PP), poly(butylene)succinate (PBS) and polydimethylsiloxane (PDMS). The hybrid LDH materials were investigated by means of X-ray diffraction and Fourier transform IR spectroscopy resulting in the presence of contracted basal spacing over the entire variation of m. Dispersion into polymer was found to yield intermixed polymer structures regardless of either the polymer or of the alkyl chain length. PP polymer chain was able to diffuse into the interlayer space, long alkyl chains (m ≥ 14) were found to reinforce while shorter chains (m ≤ 12) induced a plasticizing effect. For PBS and PDMS, a chain-extender-type behavior was observed. The relative change in viscosity within the frequency sweep stress linear response was visualized by the Cole-Cole representation. The molecular weight change relative to polymer free of filler and obtained from the power-law of the zero-shear viscosity η′0 was found to be linearly dependent of the basal spacing increase in the three cases. Such cross-study using XRD and melt polymer rheology was able to unravel the attritive or plastizicing role of the organoclay as function of the basal spacing expansion in the intermixed polymer structure, and to respond whether LDH interleaved platelets were of interest for polar and non-polar polymer and finally to predictively monitor the interfacial attrition by the alkyl chain length of the surfactant molecule tethered to the LDH platelets.