The work presented in this thesis is divided into three distinct chapters covering the chemistry high-nuclearity palladium cages, the many structures of Najera's catalyst compounds and the crystal structures of molecular tweezers and their compounds. The o-palladated, chloro-bridged dimers [Pd2-phenylpyridine(-H) -u-Cl]2 and [pdN,N-dimethylbenzylamine(-H)-Cl]2 react with cyanuric acid in the presence of base to afford closed, chiral cage-molecules in which 12 organo-Pd(11) centres, located in pairs at the vertices of an octohedron, are linked by four tetrahedally arranged cyanurator(3-) ligands.