The intermolecular interactions and microscopic miscibility of the lipid bilayers of single component and binary mixtures with high content of saturated fatty acids were investigated by 2H- and 31P-NMR for phosphatidylcholine (PC), phosphatidylethanolamine (PE), phosphatidylglycerol (PG) and cardiolipin (CL). Their glycerol backbones were selectively deuterated by biosynthesis and chemical synthesis. Deuterium quadrupole splittings and phosphorus chemical shift anisotropies provided the consistent information for the molecular miscibility of each phospholipids. PE was found to be completely miscible with PG and CL. Since deuterium quadrupole splittings and phosphorus chemical shift anisotropy are identical for two components in the mixed bilayer, the dynamic structure from the glycerol backbone to phosphate group should be uniform in the binary mixture of these phospholipids. In contrast to PE, PC was not fully miscible with PG and CL at molecular resolution. The dynamic structure from the glycerol backbone to phosphate group is different for two components in the binary mixed bilayers. In the case of the mixed bilayers of PC and PE, both phospholipids are microscopically immiscible with each other. Thus, while PE, PG and CL can adapt to a new situation to form a uniform dynamic structure in mixed bilayers, PC has no ability for adaptation. The molecular miscibility in lipid bilayers was shown to depend on the molecular species and the nature of the molecular interactions. The biological significance of this result was discussed.