This review generalizes diverse computational NMR studies of different natural products involving true alkaloids (indole, quinolizidine, pyrrolizidine, piperidine, indolizidine, quinoline, isoquinoline, indoloquinoline, and guanidine alkaloids), pseudoalkaloids (terpenes and steroids), quinones, lactones, lactams, flavonoids, and many others. The diverse computational protocols employed in each particular case are thoroughly discussed with a special emphasis on their structural and stereochemical applications. The bibliography includes 165 references.