Petrosamine (1)—a colored pyridoacridine alkaloid from the Belizean sponge, Petrosia sp., that is also a potent inhibitor of acetylcholine esterase (AChE)—was investigated by spectroscopic and computational methods. Analysis petrosamine-free energy landscapes, pKa tautomerism, revealed an accurate electronic depiction molecular structure 1 as di-keto form, with net charge q = +1, rather than di...