An investigation of the effects of a controlled microenvironment on reactivity has been carried out by the synthesis and study in organized monolayers of surfactant molecules containing photochemically reactive chromophores. Reactions where substantial environmental effects have been observed include the cis-trans isomerization of olefins, ketone photoeliminations, ligand substitution processes, excimer and photodimer formation, and photoredox reactions. Both reactions occurring within the organized assemblies as well as interfacial phenomena have been investigated. Results obtained in these studies suggest possible extensions and applications for the development of new catalyst systems, biological models and controlled syntheses.