Molecular ferroelectrics with excellent piezoelectricity have gained much popularity for their mechanical flexibility, structural diversity, chemical tunability, and environmental friendliness. Over recent years, a series of high-performance molecular ferroelectrics have been synthesized with piezoresponse, approaching some typical inorganic piezoelectric ceramics. This chapter will briefly review molecular ferroelectrics in various piezoelectric forms. We will summarize the strategies expounded in some outstanding works, hoping to design application-oriented and performance-enhanced piezoelectric materials with great potential as candidates for the next-generation micromechanical and biomechanical devices.