Dye-doped deoxyribonucleic acid-surfactant films have been prepared by an intercalation method and their optical properties have been investigated. Coumarin 1 (C1), known as a neutral laser dye, can be successfully incorporated in deoxyribonucleic acid-surfactant films by immersing them in aqueous dye solution. About 6 wt% C1 can be doped in samples when the immersion time is 86400 s. C1-doped samples show pronounced optical absorption and photoluminescence bands. Not only hydrophobic-hydrophobic interactions but also molecular structures of dyes play prominent roles in the formation of neutral dye-doped deoxyribonucleic acid-surfactant films. It is surmised that C1 stays inside the double helix of deoxyribonucleic acid (DNA) and/or between the alkyl groups of surfactants.