This dataset was generated to support the investigation of multiphase polymeric coacervates as functional soft materials and catalytic microenvironments. The data encompass the structural, colloidal, and functional characterization of coacervates formed by the surfactant cetyltrimethylammonium bromide (CTAB), the polycation poly(diallyldimethylammonium chloride) (PDADMAC), and the polyanion poly(acrylic acid) (PAA). The scope of the dataset includes small-angle X-ray scattering (SAXS) data describing the internal nanostructure of distinct coacervate phases, dynamic light scattering (DLS) measurements of polymeric coacervate micelles, and coacervate droplet size distributions in organic solvents. In addition, the dataset contains fluorescence-based kinetic data from enzymatic reactions conducted within PDADMAC–PAA coacervate droplets in organic media, using α-chymotrypsin as a model enzyme. Collectively, these data provide a comprehensive experimental basis for understanding the structure–property–function relationships in multiphase coacervate systems and their application in enzyme stabilization and catalysis in non-aqueous environments.