Macrocyclic lactones have redolent characteristics of muscones that originate from the rectal musk organs of the musk deer. These lactones are the primary raw material in the flavor and fragrance industry and are also found within the cyclic frameworks of various bioactive molecules. Due to great demand, many efforts have been made for their synthesis; however, strategies generating a large number of macrocyclic analogues from renewable resources have not been fully realized and are urgently required. Here, we outline a sustainable, straightforward, and eco-friendly approach to synthesize high-valued macrocyclic lactones utilizing olive oil under greener reaction conditions. The outlined method allows us to turn biomass into valuable 12- to 29-membered lactones and dilactones.