Sheeted or fibrous piezoelectric devices have been recently developed as actuators or sensors. These light and flexible devices are expected to create many innovative methods for the vibration control of structures. In this paper, we discuss the active control of vertical and horizontal micro-vibration of an architectural frame structure using Macro Fiber Composites (MFCs). MFCs are sheeted piezoelectric devices constructed with fibrous piezoceramics that can produce relatively higher forces than other sheeted piezoelectric devices. We arranged MFCs at the lower flange of both ends of a beam as actuators. By the expansion and contraction of the MFC actuators, bending moments act at both ends of the beam. The synchronized movements of the MFC actuators control the vertical vibration of the beam or slab. The opposite phase movements control the horizontal vibration of the frame structure. MFCs used as sensors are arranged at arbitrary positions on the lower flange surface. An experiment of vertical and horizontal vibration control on a scaled frame model is conducted and the results show that the control method effectively minimizes the resonant vibration. A vertical vibration control test on a real architectural structure is also conducted. The MFCs are arranged at the ends of two beam-spanning girders. Consequently, the vertical floor vibration of 0.04 m/s2 at 8.5 Hz at the center of the grid was reduced to 0.01 m/s2 or about −12 dB.