High-performance nanocomposites of NaCMC with GO are produced by solution casting. FESEM images reveal a good homogeneous dispersion of GO in the NaCMC matrix. The composite formation is facilitated by H-bonding interaction between GO and NaCMC. Tg of the composites increases with increasing GO concentration. The storage modulus (G′) exhibits a maximum 174% increase over NaCMC at 1 wt% GO. The mechanical properties of the composites exhibit highest increase of tensile stress and Young's modulus of 188 ± 4% and 154 ± 11%, respectively, for 1 wt% GO. Analysis of Young's modulus (Ey) data using the Halpin-Tsai equation suggests that the Ey data are close to the unidirectional orientation at >0.5 wt% GO, indicating more efficient load transfer at these compositions.