Neuroscience has further increasingly applied nanotechnology strategies to develop innovative biocompatible nanotools with unprecedented abilities for improving neuronal network formation and signaling, thus achieving better diagnosis and treatment of various neurological diseases. These nano-scaled materials with various structures and morphologies exhibit tailored functions, making them interact with different bio-systems in a particular manner. Several nano-based tools have been shown to promote cell adhesion and growth, both in vitro and in vivo, as biocompatible substrates. Various flexible, thermally, and electrical conductive 2D and 3D nanocomposites have been shown to be extremely useful for tissue regeneration and repair. Accordingly, nanomaterial-based strategies have been employed for the fundamental studies of neurological diseases. They can further serve as a potential candidate for the theranostics of nerve injury and neurodegenerative diseases in clinical practice. In our lab, we develop and test new generations of nano-engineered tools for restoring impaired neurovascular communication. This approach promises to provide much-needed breakthroughs in developing therapeutic strategies to treat brain diseases.