Schizanthus grahamii is an endemic Chilean plant that is known to contain tropane alkaloids. Five new alkaloids, grahamines A-E (1-5), were isolated and characterized by extensive spectroscopic analysis. Their structures were determined to be 2-{[(3 alpha-hydroxytropo-6 beta-yl)oxy]carbonyl}-2-methyl-3-{[((6 beta-angeloyloxy)-3 alpha-yl)oxy]carbonyl}-4- phenylcyclobutanecarboxylic acid (1), 2-{[(3 alpha-hydroxytropo-6 beta-yl)oxy]-carbonyl}-2-methy1-3-{[((6 beta-tigloyloxy)-3 alpha-yl)oxy]carbonyl}-4-phenylcyclobutanecarboxylic acid (2), 1-methyl-2-{[(3 alpha-hydroxytropo-6 beta-yl)-oxy]carbonyl}-4-{[((6-angeloyloxy)-3 alpha-yl)oxy]carbonyl}-3-phenylcy- clobutanecarboxylic acid (3), 1,2-bis{[(3 alpha-hydroxytropo-6 beta-yl)oxy]-carbonyl)-2-methyl-3-{[((6 beta-angeloyloxy)-3 alpha-yl)oxy]carbonyl}-4-phenylcyclobutanecarboxylate (4), and 1-{[(3 alpha-mesaconyloxytropo-6 beta-yl)-oxy]carbonyl}-2-{[(3 alpha-hydroxytropo-6 beta-yl)oxy]carbonyl}-2-methyl-3-{[((6 beta-angeloyloxy)-3 alpha-yl)oxy]carbonyl}-4-phenylcyclobutanecarboxylate (5).