The second example of the Ce(III)-based single-molecule magnet (SMM), which involves only one 4f electron as a spin carrier, was realized based on similar magnetostructural correlations with Tb(III)-based SMMs. The estimated energy barrier for spin flipping was Delta E/k(B) = 37(1)K, which is higher than that for the first Ce(III)-SMM, and slow magnetic relaxation was observed up to 15 K.