Coupling between electrical and mechanical phenomena is an important feature of functional inorganic materials and biological systems alike. The applications of electromechanically active materials include sonar, ultrasonic and medical imaging, sensors, actuators, and energy-harvesting technologies, as well as non-volatile computer memories. Electromechanical coupling in electromotor proteins and cellular membranes is the universal basis for biological functionalities from hearing to cardiac activity. The future will undoubtedly see the emergence of broad arrays of piezoelectric, biological, and molecular-based electromechanical systems to allow mankind the capability not only to “think” but also “act” on the nanoscale. The need for probing electromechanical functionalities has led to the development of Piezoresponse Force Microscopy (PFM) as a tool for local nanoscale imaging (Figures 1 and 2), spectroscopy, and manipulation of piezoelectric and ferroelectric materials.