Highly lattice-mismatch (over 8%) ternary InxGa1-xSb alloy directly grown on GaAs substrates was demonstrated by metalorganic chemical vapor deposition (MOCVD). The influence of growth parameters, such as growth temperature, indium vapor composition, and V/III ratio, on the film properties was investigated, and it was found that the growth temperature has the strongest effect on the surface morphology and the crystal quality of the InxGa1-xSb epilayer. An optimized growth temperature of ∼590 °C and a V/III ratio of 2.5 were used for the growth of the InxGa1-xSb epilayer on GaAs that displays a lower surface roughness. High-resolution transmission electron microscopy micrographs exhibit that InxGa1-xSb epilayer growth on GaAs was governed by the interfacial misfit dislocation growth mode. Furthermore, the variation of the intermixing layer thickness at the InxGa1-xSb/GaAs heterointerface was observed. These results provide an information of growing highly lattice-mismatched epitaxial material systems by MOCVD growth process.