Poly[9,9′‐dihexylfluorene‐2,7‐diyl)‐6,6″‐(2,2′:6′,2″‐terpyridine)] (LaPPS75) and its complexes with neodymium were synthesized and characterized. Magnetic measurements showed that the noncomplexed polymer presented a ferromagnetic contribution due to the formation of π stacking, and that in absence of those, the ferromagnetic behavior is suppressed. The pristine polymer, the complexed one and a low‐molecular‐weight model compound with the same structure of the complexed site in the parent polymer were studied. The observed behavior found is presented and discussed, the most important finding was that when a conjugated chain is used as a host for the metallic ion, an amplification of four times for the magnetization is achieved, using the same metallic content for complexed polymer and model compound for comparison. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2019, 57, 304–311

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The magnetic properties of a polyfluorene derivative, {Poly[9,9'-dihexylfluorene-2,7-yl)-3,8-(1,10-phenanthroline)]} and its complexes with neodymium ions are explored and discussed in the light of the macromolecular configuration and photophysical properties. The pristine noncomplexed material is a diamagnetic material, and the introduction of Nd atoms in the polymer leads to a paramagnetic behavior over the entire temperature range. The prominent role of the morphology is demonstrated by comparison of two forms, with different ligands to the metal: one with bulky 𝜷-diketone groups and another with small chorine as ligands. The large groups hinder interchain interaction, whereas the smaller salt forms favored interchain 𝝅-stacking, providing a better interaction of the magnetic field with the polymer backbone, resulting in enhanced magnetic properties. The form with the 𝜷-diketone groups exhibits a paramagnetic behavior whereas the one in the salt form presents ferromagnetic behavior at room temperature. This contribution brings solid confirmation to the importance of interchain interaction in the magnetic properties of conjugated polymers, opening a new way to the obtainment of magnetic conjugated polymers.