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Double-layered manganites are natural superlattices with low thermal conductivity, which is of importance for potential thermoelectric applications. The Gd2−2xSr1+2xMn2O7 (x = 0.5; 0.625; 0.75) were prepared by the solid-state reaction method. All the samples crystallize in the tetragonal I4/mmm Sr3Ti2O7 type structure. The unit cell volume and the distortion in the MnO6 octahedra increase with increasing Gd content. Their thermoelectric properties were investigated between 300 and 1200 K. All exhibit an n-type semiconducting behavior. The electrical conductivity (σ) increases while the absolute value of the Seebeck coefficient (|S|) decreases with increasing Gd content. Simultaneous increases in σ and |S| with increasing temperature are observed at temperatures approximately higher than 600 K, and the power factor reaches a maximum value of 18.36 μW/(m K²) for x = 0.75 at 1200 K. The thermal conductivity (κ) is lower than 2 W/(m K) over the temperature range of 300–1000 K for all the samples and a maximum dimensionless figure of merit ZT of 0.01 is obtained for x = 0.75 at 1000 K.