A bifunctional dysprosium(III) dimer, [Dy-2(HTPEIPOMe)(2)(OAc)(4)(NO3)(2)] (1), comprising an ALE-active (AIE = aggregation-induced emission) ligand of 2-methoxy-6-[[[4-(1,2,2-triphenylvinyl)phenyl] imino] - methyl]phenol (HTPEIPOMe), was successfully synthesized. It not only behaves as a single-molecule magnet (SMM) with an energy barrier of 168(15) K at zero field but also exhibits piezochromism during the pressing fuming cycle with switchable color, photoluminescence, and magnetic response.