The magnetic and magneto-caloric properties of (Gd1−xTbx) alloy thin films and [Gd/Tb] multilayers have been investigated. All the samples had a total thickness of 100 nm and were deposited by DC sputtering. By changing the composition of the system, the ordering temperature (Tc) and the magnetic entropy changes of the compounds could be tuned. The results show that the Tc of the alloy thin films is close to 270 K for x = 0.2. Moreover, creating [Gd/Tb] multilayers with the same thickness and concentration of the studied Gd80Tb20 alloy film enables to strongly increase the relative cooling power, and reach values twice as big as from the corresponding alloys. These results suggest that nanostructuring of [Gd/Tb] multilayers may be a promising route to tailor the magnetocaloric response of materials.