An in-situ composite film of a thermotropic liquid crystalline polymer (LC3000)/polypropylene (TLCP/PP) was produced using the extrusion cast him technique. The compatibilizing effect of thermoplastic elastomers, styrene-ethylene butylene-styrene (SEBS), maleic anhydride grafted SEES (MA-SEBS), and maleic anhydride grafted polypropylene (MA-PP) on the mechanical properties and morphology of the TLCP/PP composite films was investigated. It was found that SEES provided a higher value of tensile modulus than MA-SEES, which in turn was higher than MA-PP, despite the expected stronger interaction between the MA chain and TLCP. The observation of the morphology under optical and scanning electron microscopes suggested that all three compatibilizers helped improve the dispersion of the TLCP fibers and increased the fiber aspect ratio to a different extent. The fractured surface of the specimens showed more fiber breakage than pull-out when a compatibilizer was added, which suggested the improvement of interfacial adhesion. The surface roughness of fibers with an added elastomeric compatibilizer may also provide mechanical interlocking at the interface. It is suggested that the increase in the viscosity ratio of TLCP/PP due to the added elastomeric compatibilizer, SEES and MA-SEBS, compared with the thermoplastic compatibilizer, MA-PP, is more effective in improving the composite mechanical properties.