The spontaneous interaction of molecules/molecular entities featuring distinct properties through non-covalent interactions lead to the formation of molecular assemblies called 'superstructures'. The microscopic and macroscopic properties of such superstructures generally depend on the nature of the constituent molecules. For example, shape anisometric molecules usually composed of rigid and flexible moieties tend to self-assemble and form liquid crystal (LC) phases (mesophases).In this book, Chapter I describes about LCs and applications. Chapter II comprises with the synthesis and characterization of self-assembly homomeric dipeptides and bisamides derived from naturally occurring amino acids. They are formed by covalently linking phenyl rings substituted with alkoxy tail/s through a self-complementing spacer derived from amino acid residue/s (L/D-alanine, L/D-leucine, L/D-valine). The nature of the constituent amino acid residue/s, influence their LC behavior, in particular polar columnar phase involving hydrogen (H) bonding. Chapter III describes the synthesis and thermal behavior of non-symmetric dimers and Chapter IV about bidentate ligands and their Cu/Pd(II) metal complexes