Here we have investigated the influence of the antenna group position on both the formation of chiral amphiphilic Eu
III‐based self‐assemblies in CH
3CN solution and, on the ability to form monolayers on the surface of quartz substrates using the Langmuir–Blodgett technique, by changing from the 1‐naphthyl ( 2(
R) , 2(
S) ) to the 2‐naphthyl ( 1(
R) , 1(
S) ) position. The evaluation of binding constants of the self‐ assemblies in CH
3CN solution was achieved using conventional techniques such as UV/Visible and luminescence spectroscopies along with more specific circular dichroism (CD) spectroscopy. The binding constants obtained for EuL , EuL
2 and EuL
3 species in the case of 2‐naphthyl derivatives were comparable to those obtained for 1‐naphthyl derivatives. The analysis of the changes in the CD spectra of 1(
R) and 1(
S) upon addition of Eu
III not only allowed us to evaluate the values of the binding constants but the resulting recalculated spectra may also be used as fingerprints for assignment of the chiral self‐assembly species formed in solution. The obtained monolayers were predominantly formed from EuL
3 (≈85 %) with the minor species present in ≈15 % EuL
2 .
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