Approximately two billion people worldwide lack access to clean drinking water, negatively impacting national security, hygiene, and agriculture. Atmospheric water harvesting (AWH) is the conversion of ambient humidity into clean water; however, conventional dehumidification is energy-intensive. Improvement in AWH may be achieved with elastocaloric cooling, using temperature-sensitive materials in active thermoregulation. Potential benefits, compared to conventional desiccant wheel designs, include substantial reductions in energy use, size, and complexity. A nickel–titanium (NiTi) elastocaloric water harvester was designed and compared with a desiccant wheel design under controlled conditions of relative humidity, air volume, and power. In a 30 min interval, the NiTi device harvested more water on average at 0.18 ± 0.027 mL/WH, compared to the 0.1567 ± 0.023 mL/WH of the desiccant wheel harvester. Moreover, the NiTi harvester required half the power input and was thermoregulated more efficiently. Future work will focus on mechanical design parameter optimization. Elastocaloric cooling is a promising advancement in dehumidification, making AWH more economical and feasible.