For thousands of years, Nature has been considered to be essential to human beings for the treatment of their diseases. Amphibians are an important component of the Animal Kingdom and have played a significant role in sourcing many active and some therapeutic compounds. The secretions of amphibians act as defensive substances spreading out over their skins to protect them from predator attack and infections by microorganisms. These skin secretions represent a spectacular library of bioactive molecules, including peptides. In recent years, many different kinds of antimicrobial and pharmacological peptides have been isolated from amphibian skin secretions and some of these are providing potential human therapeutic leads. In the course of this research, genomic and proteomic techniques have been used to investigate the bioactive peptides from the skin secretions of four species of frog: the Central American red-eyed leaf frog, Agalychnis callidryas; the Peruvian purple-sided leaf frog, Phyllomedusa baltea; the European edible frog, Pelophylax kl. esculentus; the Fujian large-headed frog, Limnonectes fujianensis. The peptides isolated in these studies could be divided into two antimicrobial peptide families (balteatide and QUB3276) and two pharmacological peptide families (the bombesin-related peptides and AcT-2). The latter peptide was found to have both antimicrobial and pharmacological functions. Synthetic replicates of each peptide were prepared and used in an extensive range of biological assays.These discoveries of novel peptides from amphibian skin secretions have enriched our knowledge of bioactive peptides from this source and may provide the basis for several drug development programmes.