The complexation of the bismalonamide ligand 2,2′-[1,2-phenylenebis(methylene)]bis(N,N,N′,N′-tetraethylmalonamide) (L), bearing two C-alkylated N,N,N′,N′-tetraethylmalonamide groups, onto an ortho-xylylene [C 6 H 4 (CH 2 ) 2 ] platform with trivalent lanthanides was investigated, both in solid and solution states. The crystal structures [Nd 2 (NO 3 ) 6 L 2 ]·(CH 3 CN) 3 (2), [Nd 2 (NO 3 ) 4 L 2 ]·[Nd(NO 3 ) 5 ]·(CH 3 CN) 1.5 (3), Ce(NO 3 ) 3 L 2 (4), and [NdL 2 ]·(ClO 4 ) 3 ·C 2 H 5 OH (5) were analyzed by single-crystal X-ray [a]