A redox active dinuclear complex [Yb(tta)₂(L¹)(L²)]₂·1.4(CH₂Cl₂) displays single molecule magnet behaviour with M_J = ±7/2 ground state. The anisotropic barrier Δ is evaluated by the three dc data fit, ac analysis and emission spectrum demonstrating the correlation between magnetic and optical properties.

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^IIIwere 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)₃units (hfac⁻=1,1,1,5,5,5‐hexafluoroacetylaconate), efficient NIR‐CPL activity is observed. Moreover, the specific crystal field around the Yb^IIIinduces 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.