We used stereolithography to print polymer nanocomposite samples of stimuli-responsive spin crossover materials in the commercial photo-curable printing resins DS3000 and PEGDA-250. The thermomechanical analysis of the SLA-printed objects revealed not only the expected reinforcement of the polymer resins by the introduction of the stiffer SCO particles, but also a significant mechanical damping, as well as a sizeable linear strain around the spin transition temperatures. For the highest accessible loads (ca. 13–15 vol.%) we measured transformation strains in the range of 1.2–1.5%, giving rise to peaks in the coefficient of thermal expansion as high as 10⁻³ °C⁻¹, which was exploited in 3D printed bilayer actuators to produce bending movement. The results pave the way for integrating these advanced stimuli-responsive composites into mechanical actuators and 4D printing applications.