A series of optical properties of some natural dyes are reported and discussed. The studied bio-dyes were extracted from different spices and showed interesting photosensitive properties. Thin films were obtained by solution casting of complexes obtained by dissolving the studied dyes in deoxyribonucleic acid (DNA). Purely biological, biodegradable materials were obtained and spectrally characterized. Also their hydrophilic-lipophilic balance was established, and the color analysis was performed. The obtained results showed that DNA-natural dye complexes exhibit an interesting potential for application in photonics and may serve as an eco-friendly alternative for hardly degradable and highly polluting synthetic polymers and dyes.