Vapor-grown carbon nanofibers were filled into poly(ethylene-co-vinyl acetate) through solution mixing to achieve electrical-active two-way shape memory. The vapor-grown carbon nanofiber/poly(ethylene-co-vinyl acetate) nanocomposites were systematically and explicitly investigated through combined analytical techniques. Experimental results showed an increase in crystallization temperature ( Tc) and a decrease in melting temperature ( Tm) as the vapor-grown carbon nanofiber concentration in the nanocomposites increased. This result indicates that carbon nanofibers can act as nucleating agents during crystallization but may hinder the formation of thermodynamically stable crystals. The nanocomposites had a higher modulus but a lower strength than pure poly(ethylene-co-vinyl acetate). In two-way shape memory testing, a decrease in reversible strain and shape recovery occurred in the nanocomposites. Nevertheless, obvious two-way shape switching was observed in all samples during cyclic heating and cooling. The nanocomposite with 15% vapor-grown carbon nanofibers could be electrically heated rapidly and uniformly because of the high conductivity of vapor-grown carbon nanofibers and their uniform distribution in the matrix. Finally, the electrical-active two-way shape memory effect was achieved. This work contributes to the design of electrical-active two-way shape memory polymers in device applications for advanced functions.