The temperature dependence of the elastocaloric (eC) effect in natural rubber (NR) has been studied. This material exhibits a large eC effect over a broad temperature range from 0 °C to 49 °C. The maximum adiabatic temperature change (ΔT) occurred at 10 °C and the behavior could be predicted by the temperature dependence of the strain-induced crystallization (SIC) and the temperature-induced crystallization (TIC). The eC performance of NR was then compared with that of shape memory alloys (SMAs). This study contributes to the SIC research of NR and also broadens the application of elastomers.