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In this work, a functionalized hybrid Al2O3-GO was fabricated and introduced into trans-1,4-polyisoprene (TPI) matrix as a new filler. The incorporation of the hybrid optimized the heat resistance, mechanical strength, and fracture toughness of the composites simultaneously. The ultrathin GO shells at Al2O3-TPI interfaces were considered to be the main reason for the enhancement. They effectively enhanced the interfacial interaction of the Al2O3-GO/TPI nanocomposites, thus greatly improved the thermodynamic properties of the TPI. The mechanical, thermal, and shape memory properties of nanocomposites were characterized through systematic tests from microscale to macroscale. According to the experimental results, the nanocomposite samples with GO (0.9 wt%) and Al2O3 nanoparticles (1.2 wt%) show the best thermal and mechanical properties in comparison with other samples, and a good shape memory property was obtained or realized in the fabricated nanocomposites. We believe this new and effective approach may open a novel interface design strategy for developing high performance composites. Keywords: Al2O3-GO nanohybrids, Polymer nanocomposite, Thermodynamic properties, Shape memory