Continuing work on Labiatae family terpenoids, we report diterpenoids from Amuraus akhdarensis (syn. Origanum akhdarensis) and Amuracus pampanini (Libya-grown). Amuracus, once assimilated into Origanum, was proposed for restoration as a separate genus; this chemical investigation of secondary metabolites aimed to support taxonomic classification. From A. akhdarensis, three diterpenes—akhdarenol (1), akhdardiol (2), akhdartriol (3)—were isolated, along with triterpenes (oleanolic/ursolic acids) and flavonoid cirsimaritin. From A. pampanini, akhdardiol was the only diterpene, plus triterpenes (oleanolic/ursolic acids, uvaol) and flavonoids (7-O-methyl-acacetin, 5-O-desmethyl-nobiletin). Structural elucidation (NMR, IR, MS, chemical reactions) assigned akhdarenol as isopimara-7,15-dien-19-ol (identical to a fungal product, confirming stereochemistry), akhdardiol as isopimar-15-en-8β,19-diol (new natural product), and akhdartriol as isopimar-15-en-8β,11α,19-triol. No diterpenes were found in Origanum heracleoticum (Sicilian). These findings support Amuracus-Origanum differences, justifying genus separation.