The need for eco‐friendly cooling materials and material recycling are two urgent challenges to address. In this paper, the role of the ground tyre rubber treatment (cryo‐grinding and devulcanization) is investigated on the tensile and elastocaloric properties of Natural rubber (NR)/ ground tyre rubber (GTR). The GTR particles that are sieved (<63µm) and devulcanized by microwave irradiation (1 min at 800Watts) exhibit a low network chain density (0.53 × 10−4 mol.cm−3) resulting from crosslinks breakage and rubber chains scission, as supported by FTIR showing a decrease of S─S, C─S, and C─C bonds. The NR/GTR blends show a high elastocaloric effect as compared to the pristine NR, which can be ascribed to the high content of carbon black in the GTR (52 wt.%) and also the high level of devulcanization of the GTR. NR/GTR blends reach a heating of +8 °C and a cooling of >−6 °C, resulting in a material's coefficient of performance COPmat = 2.8–3 compared to 2.6 for the pristine NR. The concomitant effect of cryogrinding and microwave devulcanization is proposed as a way to improve the tensile and elastocaloric properties of natural rubber/waste rubber blends for their possible integration into elastocaloric devices for heating/cooling applications.