There are subtle mechanisms at work in nature to maintain a balance in the interactions between plants and animals. The production of secondary metabolites is one of the key strategies utilized by plants to minimize their over-exploitation. The ‘lily borer’ moth Brithys crini poses a considerable challenge to Amaryllidaceaous plants owing to the devestation it can cause during the larval stage of its development. This, despite the fact that the Amaryllidaceae is richly endowed with an assortment of isoquinoline alkaloids which exhibit a diverse array of biological properties, particularly cytotoxicity-related effects. In this study, laboratory-maintained larvae of B. crini were periodically fed fresh leaves of Crinum moorei during the September to November infestation period in Pietermaritzburg, South Africa. Solvent extracts of the plant leaves, moth larvae and larvae excrement material were then prepared and subjected to HPLC and LC-MS analyses. The presence of several alkaloids, including cherylline and ambelline, in all three extracts was ratified via HR-MS and NMR analyses. The identification of ambelline is noteworthy since it has not been reported in previous studies of C. moorei. Toxicity related criteria are also considered based on the present detection of alkaloids in B. crini larvae material, as well as precedence for their association with other known insect predators of the Amaryllidaceae.