This thesis describes the synthesis and characterisation of novel cyclopalladated metallomesogens from four principal N-functionalised mesogenic ligands:(i) 4-alkyloxy-N- (4' -alkyloxybiphenyl)benzylidene, (H) terephthalylidene-bis-4-N-4' -alkyloxybenzylidene, (iii) bis( 4-alkoxybenzylidene-l ,4-phenylenediamine and (iv) 3, 6 bis- (alkyloxyphenyl)pyridazine). The ligands have been studied to determine their liquid crystalline behaviour and the phase behaviour is reported for the terephthalylidene-bis-4-N-4' -alkyloxybenzylidene series and for the 3, 6 bis-(alkyloxyphenyl)pyridazine series since no comprehensive study of either system has been reported in the literature. The co-ordination chemistry of these ligands is reported. The regiospecificity of the cyclopalladation reaction for the terephthalylidene-bis-4-N-4' -alkyloxybenzylidene and 3, 6 bis(alkyloxyphenyl)pyridazine series has been established and the influence of the primary cyc1opalladationstep on secondary cyclopalladationhas been examined. The co-ligands acetylacetonate, undecane-5,7 -dione, pentandecane-7,9-dione, nonadecane- 9,1O-dione, 2,2,6,6 tetra-methyl-heptane-3,5-dione and cyclopentadienylide have been employed to enable elaboration of the geometry of the organopalladium complexes giving diversity to the structure and physical properties of these materials.