Novel polyacrylamide gel electrolytes (PGEs) doped with nano carbons with enhanced electrochemical, thermal, and mechanical properties are presented. Carboxylated carbon nanotubes (fCNTs), graphene oxide sheets (GO), and the hybrid of fCNT/GO were embedded in the PGEs to serve as supercapacitor (SC) electrolytes. Thermal stability of the unmodified PGE increased with the addition of the nano carbons which led to lower capacitance degradation and longer cycling life of the SCs. The fCNT/GO-PGE showed the best thermal stability, which was 50% higher than original PGE. Viscoelastic properties of PGEs were also improved with the incorporation of GO and fCNT/GO. Oxygen-containing functional groups in GO and fCNT/GO hydrogen bonded with the polymer chains and improved the elasticity of PGEs. The fCNT-PGE demonstrated a slightly lower viscous strain uninform distribution of CNTs in the polymer matrix and the defects formed within. Furthermore, ion diffusion between GO layers was enhanced in fCNT/GO-PGE because fCNT decreased the aggregation of GO sheets and improved the ion channels, increasing the gel ionic conductivity from 41 to 132 mS cm−1. Finally, MnO2-based supercapacitors using PGE, fCNT-PGE, GO-PGE, and fCNT/GO-PGE electrolytes were fabricated with the electrode-specific capacitance measured to be 39.5, 65.5, 77.6, and 83.3 F·g−1, respectively. This research demonstrates the effectiveness of nano carbons as dopants in polymer gel electrolytes for property enhancements.