Crosslinkable metallomesogens containing thermally reactive 1,3-diene tails are described (see Figure). These polymerizable Pd-II and Ni-II-containing liquid crystals (LCs) exhibit LC behavior more similar to their non-polymerizable n-alkoxy parent compounds than their corresponding acrylate derivatives. The diene monomers can be thermally crosslinked in their LC states without significant degradation of their redox-sensitive metal centers via non-radical [4 + 2] intermolecular cycloaddition.