The incorporation of chiral amphiphilic lanthanide-directed self-assembled Nd III complexes (Nd.1 3 and Nd.2 3 ) into stable Langmuir monolayers, and the subsequent Langmuir-Blodgett film formation of these, is described. The photophysical properties of the enantiomeric pair of ligands 1 and 2 in the presence of Nd(CF 3 SO 3 ) 3 were also investigated in CH 3 CN solutions using UVVis, fluorescence, lanthanide luminescence spectroscopies. Analysis of the resulting selfassembly processes revealed that two main species were formed in solution