In the present research, results are presented regarding the anelasticity of 99.999% pure aluminum thin films, either deposited on silica substrates or as free-standing sheets obtained by cold rolling. Mechanical Spectroscopy (MS) tests, namely measurements of dynamic modulus and damping vs. temperature, were performed using a vibrating reed analyzer under vacuum. The damping vs. temperature curves of deposited films exhibit two peaks which tend to merge into a single peak as the specimen thickness increases above 0.2 m. The thermally activated anelastic relaxation processes observed on free-standing films are strongly dependent on film thickness, and below a critical value of about 20 m two anelastic relaxation peaks can be observed; both ...