In this article, we review some of our recent work on the development and study of the properties of self-organizing supermolecular liquid crystalline dendritic materials. Prior to this purpose, the state of the art in the field of molecular design, structure and properties of liquid-crystalline dendrimers (LCDs) will be briefly reviewed, and illustrated by a selection of pioneering examples. The first type of LC dendrimer takes into account the location of their functional elements (mesogens) in the periphery of the macromolecules and its topology of attachment, and the nature of the mesogen. We will show how functionality can be in-built into such materials so that self-organising functional systems can be created. Side-chain liquid-crystalline dendrimers exhibiting lamellar, columnar and nematic phases are shown. The mechanism of mesophase formation (mesogen interaction versus microphase separation) is also discussed in relation to the molecular structure (the nature of the mesogen and of the dendritic matrix, dendritic generation number). The second type of LC dendrimer introduced presents a different topology in that the mesogens are now inserted within the dendritic matrix and in the periphery. Owing to their particular constitution, it will be shown that the mesophases of the lamellar and columnar types possess unusual morphologies.