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A hexanuclear Nd (III) complex {[Nd6(HL)2L2X2(NO3)8(EtOH)6]·(EtOH)(H2O)3} (H2L = 2,3‐dihydroxybenzaldehyde‐4‐aminoantipyrine; H2X = 2,3‐dihydroxy benzaldehyde) has been designed, synthesized, and evaluated for antitumor and antifungal activity. Single‐crystal X‐ray diffraction analysis indicates Nd (III) complex has a trinuclear cluster structure, which further forms a hexanuclear monomer through two bridging ligands L2−. There are π–π interactions and a lot of intramolecular hydrogen bonds between monomers. Antitumor activity of Nd (III) complex against human hepatocellular carcinoma SMMC‐7721 cells has been studied by 3‐(4,5‐dimethyl‐2‐thiazolyl)‐2,5‐diphenyltetrazolium bromide (MTT) assay and morphology observation. The IC50 value of Nd (III) complex ranges from 4.02 to 4.85 μM, much smaller than that of clinical drug (gemcitabin) and free ligand (H2L), which is consistent with its high inhibition rate of 90%. Inhibitory zone of 26 mm reveals the significant antifungal activity of Nd (III) complex against Candida albicans. [ABSTRACT FROM AUTHOR]