Molecular spin-crossover (SCO) complexes are phase-change materials that develop large spontaneous strains across the thermally induced phase transition, which can be advantageously used in designing soft actuators. Herein, a bilayer bending cantilever, made of thermoplastic polyurethane (TPU) with embedded [Fe(NH2trz)3](SO4) SCO particles (25 wt%), is presented. The proposed actuator is fabricated by blade casting an SCO@TPU layer on a conducting Ag@TPU film to convert electrothermal input into mechanical response. Experiments are conducted to characterize the curvature of bilayer beams, which is then further analyzed using the Euler–Bernoulli beam theory. The beam curvature change, free transformation strain, and effective work density associated with the SCO are 0.11 mm−1, 1.6%, and 1.25 mJ cm−3, respectively. Further, the open- and closed-loop response of the actuator is investigated using a custom-built setup. The open-loop identification suggests that the actuator gain increases monotonously when the control current increases. This natural adaptive character can explain the drastically diminished response time in closed-loop proportional–integral–derivative control experiments (2–3 s). Finally, tracking experiments are carried out to evaluate the robustness of the actuator with and without payloads. The results for 30 240 endurance cycles reveal a mean positioning error of 0.8%.