n this work, coixalkyne A (1), a natural polynuclearcalcium complex with a novel cross-shaped molecular architecture,was isolated from Coix lacryma-jobi L. along with the undescribedanalogue coixalkyne B (2). Their structures were identified bymeans of NMR spectroscopy, ECD calculations, and single-crystalX-ray diffraction. It is noteworthy that the calcium ligands of 1 aswell as compound 2 possess rare terminal alkynes and a nor-carbonsesquiterpene (C14) framework. The antihyperuricemic activity ofC. lacryma-jobi and xanthine oxidase (XOD) inhibitory effects of1−2 were elucidated by in vivo and in vitro assays, while thepossible mechanism of action was suggested by molecular docking.Different from the reported chemical synthesis and protein calciumcarriers, the discovery of compounds 1 and 2 provided new prooffor the natural calcium metallophore in plants with xanthine oxidase inhibitory activity.