The photoresponsive nature of azobenzene-containing polymers has wide potential application for fast, miniature shape change with a minimal need for mechanical interference. This presentation explores the vibrational nature of two polymers and their monomer precursors through infrared and Raman studies. Studies on two related crosslinked polymers will be presented. The basic repeat unit of the first polymer is 4-hexyloxy-4'-(6-acryloyloxyhexyloxyazobenzene) with 4,4'-bis(6-acyloyloxyhexyloxyazobenzene) as a crosslinker while the second polymer has the same crosslinker but 4-ethyloxy-4'-(6-acryloyloxyhexyloxyazobenzene) is the basic repeat unit. Theoretical vibrational studies were performed for the polymer precursors and these results are later compared to steady state FTIR and Raman spectra. From the spectra of these precursors the vibrational assignments of the polymers are well understood and will be presented in detail. It has also been demonstrated that a macroscopic photomechanical effect results from illumination with 442 nm laser excitation. This effect results from a reversible photoisomerization of the azo-bonds inherent in each polymer. This photoisomerization also leads to measurable changes in both the infrared and Raman spectra. These spectroscopic changes will also be a topic of discussion.