Interactions between the binary combination of dimethyltetradecylammoniopropanesulfonate (TPS) and L-α-phosphatidylcholine (PC), 1,2-didecanoyl-sn-glycero-3-phosphocholine, and 1,2-dipalmitoyl-sn-glycero-3-phosphocholine in the aqueous bulk phase were evaluated with the help of pyrene fluorescence (I 1 /I 3 ) measurements by studying the aggregation processes of TPS in pure water and in the presence of 7-36 µM of fixed concentrations of each lipid. The fluorescence measurements showed that TPS monomers undergo two kinds of aggregation process, which were identified by the three breaks. The first break, C 1 , and the second, C 2 , indicated the onset and completion of bilayer solubilization, respectively, on the incorporation of TPS monomers into the bilayer assemblies, which led to bilayer solubilization in the form of mixed micelles. This process was not clearly visible in the presence of PC, whereas some kinds of structure transitions were observed upon the incorporation of surfactant monomers. The partition coefficient (K), which defines the degree of partitioning of surfactant monomers into the bilayers with respect to the aqueous medium, was evaluated. A high K value of TPS-lipid aggregates indicated stronger interactions between surfactant and bilayer assemblies of lipid. The K values determined for the three phospholipids are close to each other, which indicates that K values do not depend on the hydrocarbon chain length of the phospholipid but of the surfactant used.