Peptides have emerged as a therapeutically important class of drugs and offer the advantage of great specificity, potency and low toxicity. Short circulation half-life, poor proteolytic stability and bioavailability have however prevented them from becoming a mainstream source of drug candidates. Dendrimers are versatile, derivatizable, well-defined branched synthetic macromolecules with promising properties for a variety of applications in technology and medicine. Combining therapeutic peptides with dendrimers represents a promising approach to overcome bioavailability limitations, while at the same time introducing novel pharmacological and biophysical properties. The impact of the dendritic structure and multivalency on potency, selectivity, bioavailability and overall pharmacology will be studied on nicotinic acetylcholine and oxytocin/vasopressin G-protein coupled receptors, two important biomedical targets. A synthetic strategy based on efficient ligation chemistry and combinatorial assembly of building blocks will form the platform for the assembly of diverse multifunctional peptide dendrimers. These peptide dendrimers will undergo detailed structural, biophysical and pharmacological characterization for their use as diagnostic tools and therapeutics.