Novel robotic, bioelectronic, and diagnostic systems require a variety of compact and high-performance sensors. Among them, compact three-dimensional (3D) vector angular encoders are required to determine spatial position and orientation in a 3D environment. However, fabrication of 3D vector sensors is a challenging task associated with time-consuming and expensive, sequential processing needed for the orientation of individual sensor elements in 3D space. In this work, we demonstrate the potential of 3D self-assembly to simultaneously reorient numerous giant magnetoresistive (GMR) spin valve sensors for smart fabrication of 3D magnetic angular encoders. During the self-assembly process, the GMR sensors are brought into their desired orthogonal positions within the three Cartesian planes in a simultaneous process that yields monolithic high-performance devices. We fabricated vector angular encoders with equivalent angular accuracy in all directions of 0.14°, as well as low noise and low power consumption during high-speed operation at frequencies up to 1 kHz. Directional anisotropic sensors, transducers, and actuators are essential for the next generation of electronic devices a...