Shape memory alloys (SMAs) can recover their original shape after deformation when heated above a specific transformation temperature. This study investigates the induction of the two-way shape memory effect (TWSME) in SMA films through laser surface treatment. Ti50Ni40Cu10 SMA films with thicknesses of 20–40 μm were fabricated using the melt-spinning method and subjected to laser irradiation under varying conditions. The effects of film thickness and laser parameters on actuation characteristics and crystalline structure were evaluated. The results demonstrate the successful induction of TWSME in the laser-treated SMA films, with actuation capability depending on the balance between the modified and unmodified layers through the thickness. X-ray diffraction analysis reveals the presence of residual martensitic phase in the laser-treated specimens, contributing to the TWSME. Optimal actuation is achieved with a relatively thick modified layer while maintaining sufficient unmodified material for recovery to the memorized shape. This study provides insights into the laser-induced TWSME in SMA films and its potential applications in microactuators, where bidirectional actuation without external preloading is desirable.