Polyimides (PIs) have been extensively used in thin film and micro-electromechanical system (MEMS) processes based on their excellent thermal and mechanical stability and high glass transition temperature. This research explores the development of a novel multilayer and multifunctional polymer composite electro-piezomagnetic device that can function as an energy harvester or sensor for current-carrying wires or magnetic field sensing. The devices consist of four layers of composite materials with a polyimide matrix. The composites have various nanoparticles to alter the functionality of each layer. Nanoparticles of Ag were used to increase the electrical conductivity of polyimide and act as electrodes; lead zirconate titanate was used to make the piezoelectric composite layer; and either neodymium iron boron (NdFeB) or Terfenol-D was used to make the magnetic and magnetostrictive composite layer, which was used as the proof mass. A novel all-polymer multifunctional polyimide composite cantilever was developed to operate at low frequencies. This paper compares the performance of the different magnetic masses, shapes, and concentrations, as well as the development of an all-magnetostrictive device to detect voltage or current changes when coupled to the magnetic field from a current-carrying wire. The PI/PZT cantilever with the PI/NdFeB proof mass demonstrated higher voltage output compared to the PI/Terfenol-D proof mass device. However, the magnetostrictive composite film could be operated without a piezoelectric film based on the Villari effect, which consisted of a single PI-Terfenol-D film. The paper illustrates the potential to develop an all-polymer composite MEMS device capable of acting as a magnetic field or current sensor.