Neurological and psychiatric conditions pose an increasing socioeconomic burden on our aging society. Our ability to understand and treat these conditions relies on the development of reliable tools to study the dynamics of the underlying neural circuits. Despite significant progress in approaches and devices to sense and modulate neural activity, further refinement is required on the spatiotemporal resolution, cell-type selectivity, and long-term stability of neural interfaces. Guided by the principles of neural transduction and by the materials properties of the neural tissue, recent advances in neural interrogation approaches rely on flexible and multifunctional devices. Among these approaches, multimaterial fibers have emerged as integrated tools for sensing and delivering of multiple signals to and from the neural tissue. Fiber-based neural probes are produced by thermal drawing process, which is the manufacturing approach used in optical fiber fabrication. This technology allows straightforward incorporation of multiple functional components into microstructured fibers at the level of their macroscale models, preforms, with a wide range of geometries. Here we will introduce the multimaterial fiber technology, its applications in engineering fields, and its adoption for the design of multifunctional and flexible neural interfaces. We will discuss examples of fiber-based neural probes tailored to the electrophysiological recording, optical neuromodulation, and delivery of drugs and genes into the rodent brain and spinal cord, as well as their emerging use for studies of nerve growth and repair.