Works in our laboratory have shown that novel classes of light-absorbing and luminescent metal-containing molecular materials could be assembled through the use of various metal-ligand chromophoric motifs. In this presentation, various strategies for the design and synthesis of new classes of chromophoric and luminescent metal complexes will be described. A number of these metal-ligand chromophoric complexes have been shown to display rich luminescence and photofunctional behavior. The chromophoric and luminescence behavior have been studied. Correlations of the chromophoric and luminescence behavior with the electronic and structural effects of the metal complexes have been made to elucidate their spectroscopic origins. Some of these simple discrete metal complexes are found to undergo supramolecular assembly to give a variety of nanostructures and morphologies with different colors and emission properties. Subtle changes in the microenvironment, conformations and nanostructured morphologies have led to drastic changes in both the electronic absorption and emission properties of these hierarchical supramolecular assemblies. Explorations into the underlying factors that determine their spectroscopic properties and morphologies as well as their assembly processes have provided new insights into the understanding of their photophysics, structure-property-function relationships, and the interplay of the various intermolecular forces and interactions for the directed assembly of metal-containing supramolecular assemblies and soft materials. Manipulation of the electronic effects, molecular conformation, orientation and assembly has led to the control of the excited states in novel molecular materials and supramolecular assemblies. The exploration into the potential applications and functions of these light-emitting discrete metal complexes, supramolecular assemblies and polymers will also be described.