Multifunctional Helicene‐Based Ytterbium Coordination Polymer Displaying Circularly Polarized Luminescence, Slow Magnetic Relaxation and Room Temperature Magneto‐Chiral Dichroism**

The combination of physical properties sensitive to molecular chirality in a single system allows the observation of fascinating phenomena such as magneto‐chiral dichroism (MChD) and circularly polarized luminescence (CPL) having potential applications for optical data readout and display technology. Homochiral monodimensional coordination polymers of Yb III were designed from a 2,15‐bis‐ethynyl‐hexahelicenic scaffold decorated with two terminal 4‐pyridyl units. Thanks to the coordination of the chiral organic chromophore to Yb(hfac) 3 units (hfac − =1,1,1,5,5,5‐hexafluoroacetylaconate), efficient NIR‐CPL activity is observed. Moreover, the specific crystal field around the Yb III induces a strong magnetic anisotropy which leads to a single‐molecule magnet (SMM) behaviour and a remarkable room temperature MChD. The MChD‐structural correlation is supported by computational investigations.