Merocyanine compounds belong to the class of “push–pull” dyes and show multifunctional characteristics. Thus, their scope for application is ever increasing and they can be found in such widespread fields as data storage and UV-absorbing materials for food packaging. However, inherent limitations regarding long-term stability, efficiency, and processability require detailed studies on structure–property relationships. We carry out a systematic experimental and theoretical investigation of the absorption and emission spectra of dyes that vary in either chromophore length or acceptor unit. The consequent results provide information on structure-property relationships, which could be used to tailor potentially functional dyes.