The physical, thermal, structural, and mechanical properties of poly(methyl methacrylate) PMMA foils cast from solutions of toluene were investigated by differential scanning calorimetry, optical microscope, Fourier infrared spectroscopy, and dynamical mechanical analysis. The PMMA foils were prepared from a different ratio of PMMA powder with toluene solvent by the solution cast method. The surface features, glass transition temperature, and C-H bonds of foils were investigated and compared with commercial PMMA foil. The mechanical characterization of foils was examined by using static and dynamic loads in axial and transverse modes. The tensile behaviors of the commercial and as-prepared foils were investigated by using a strain rate of 0.01/s. The dynamical behavior of the foils was tested in tensile mode using 0.1 N of stress with a frequency of 1 Hz for the determination of storage, loss modulus, and damping values of the tan delta. A significant shape memory was observed in all of the prepared PMMA foils. The solution cast method allows for tuning the glass transition temperature of polymer foil that could easily integrate with the NiTi alloy phase transition temperature to fabricate a suitable composite structure. Integrating both structures will open the flexibility in bistable actuators in composite structures as a function of thermal cycles.