The connection of flexible protodendritic wedges to the bistridentate rigid polyaromatic ligand L1 provides amphiphilic receptors L5 and L6; their reduced affinities for complexing trivalent lanthanides (Ln = La, Y, Lu) in organic solvent (by fifteen orders of magnitude!) prevent the formation of the expected dinuclear triple-stranded helicates [Ln 2 (Lk) 3 ] 6+ . This limitation could be turned into an advantage because L1 or L6 can be treated with [Ln(hfac) 3 ] (Hhfac = 1,1,1,5,5,5-hexa-[a]www.eurjic.org FULL PAPER those with coordination number (CN) 7-12, typical of large lanthanide cations, have remained challenging for some time. [5,15] Pioneering work dedicated to fullerodendrimers [16] established that mesomorphism could be induced when the bulky spherical cores were coated with divergent polarised dendritic architectures, a strategy that led to the preparation of a unique discotic dinuclear lanthanidomesogen. [15d] To the best of our knowledge, there is no other report of multinuclear mesomorphic analogues despite a rich catalogue of polynuclear linear triple-stranded helicates such as [Ln 2 (L1) 3 ] 6+ , [Ln 3 (L2) 3 ] 9+ and [Ln 4 (L3) 3 ] 12+ , the cylindrical rigid cores of which make them ideal for the design of calamitic metallomesogens. [1] However, by following this strategy, lipophilic dinuclear helicates with d-block metals [Cu 2 (L4n) 2 ] 2+ (n = a, b, c) have been shown to self-organise into columnar mesophases. [13b,17] Interestingly, the connection of the long lipophilic and diverging alkyl chains to the cylindrical core drastically limited the stability of these complexes in solution, an observation that might explain the paucity of helical scaffolds in metallomesogens. To extend this approach to magnetically and optically active 4f-block cations, we connect here two different lipophilic protomesomorphic dendrons perpendicularly to the helical axis in 11 through ether links (L5) or ester bonds (L6) (Scheme 1).