The dynamics of thermal and non-thermal lattice deformation of a nanometer thick polycrystalline aluminum film has been studied by means of femtosecond (fs) time-resolved electron diffraction. We utilized two different pump wavelengths: 800 nm, the fundamental of a Ti:sapphire laser, and 1250 nm generated by a home-made optical parametric amplifier. Our data show that although coherent phonons were generated under both conditions, the diffraction intensity decayed with the characteristic times of 0.9 ± 0.3 ps and 1.7 ± 0.3 ps under 800 nm and 1250 nm excitations, respectively. Because the 800 nm laser excitation corresponds to the strong interband transition of aluminum due to the 1.55 eV parallel band structure, our experimental data indicate the presence of non-thermal lattice deformation under 800 nm excitation, which occurs on a time-scale that is shorter than the thermal processes dominated by electron-phonon coupling under 1250 nm excitation.