In this study, a polysiloxane grafted by thermotropic liquid crystal polymer (PSCTLCP) is designed and synthesized to effectively improve the processability and toughness of magnesium hydroxide (MH)/linear low-density polyethylene (LLDPE) composites. The obtained PSCTLCP is a nematic liquid crystal polymer; the liquid crystal phase exists in a temperature range of 170 to 275 • C, and its initial thermal decomposition temperature is as high as 279.6 • C, which matches the processing temperature of MH/LLDPE composites. With the increase of PSCTLCP loading, the balance melt torque of MH/LLDPE/PSCTLCP composites is gradually decreased by 42% at 5 wt % PSCTLCP loading. Moreover, the power law index of MH/LLDPE/PSCTLCP composite melt is smaller than 1, but gradually increased with PSCTLCP, the flowing activation energy of PSCTLCP-1.0 is lower than that of MH/LLDPE at the same shear rate, indicating that the sensitivity of apparent melt viscosity of the composites to shear rate and to temperature is decreased with the increase of PSCTLCP, and the processing window is broadened by the addition of PSCTLCP. Besides, the elongation at break of MH/LLDPE/PSCTLCP composites increases from 6.85% of the baseline MH/LLDPE to 17.66% at 3 wt % PSCTLCP loading. All the results indicate that PSCTLCP can significantly improve the processability and toughness of MH/LLDPE composites.Polymers 2020, 12, 911 2 of 15 low molecular weight PDMS (silicone oil) is a good lubricant for plastics [11,12]. A small amount of polysiloxane with long chain alkyl side group obviously increased the melt flow rate and reduced the processing difficulty of thermoplastic composites [13]. Moreover, it was found that the toughness of plastics composites was enhanced with the increase of PDMS loading [14]. However, PDMS is a typical liquid polymer and cannot be conveniently used in industrial production, compared with powdered processing aids.Thermotropic liquid crystal polymer (TLCP) possesses the excellent mechanical properties and lubrication for thermoplastic polymer melts [15,16]. During the melting process, the rigid TLCP macromolecules are easily oriented and arranged along the flow direction under the action of shear or tensile force, and ultimately improve the processability of thermoplastic composites [17][18][19][20].However, for TLCP, the prerequisite for improving the processability of thermoplastic composites is that the liquid crystal phase transition temperature range is consistent with the processing temperature of thermoplastics [21]. Unfortunately, at present, the melting temperature of most main chain thermotropic liquid crystal polymers is quite high and is just comparable to that of the engineering plastics with high processing temperature [22], but is not well matched with the polyolefins with lower processing temperature [23]. Therefore, it has attracted more and more attention to reduce the melting point of the thermotropic liquid crystal polymer and further to expand its application in polyolefin-based thermoplastic composites with low...