Cancer, despite being the bull's eye for the research community, accounts for a large number of morbidity and mortality. Cancer of the brain is considered the most intractable, with the least diagnosis rates, hence treatment and survival. Despite the extensive development of therapeutic molecules, their targeting to the diseased site is a challenge. Specially tailored nanoparticles can efficiently deliver drugs and genes to the brain to treat tumours and diseases. These nanotechnology-based strategies target the blood-brain barrier, the local space, or a specific cell type. These nanoparticles are preferred over other forms of targeted drug delivery due to the chances for controlled delivery of therapeutic cargo to the intended receptor. Targeted cancer therapy involves using specific receptor-blocking compounds that block the spreading or growth of cancerous cells. This review presents an account of the recent applications of nano-based cancer theragnostic, which deal in conjunct functionalities of nanoparticles for effective diagnosis and treatment of cancer. It commences with an introduction to tumours of the brain and their grades, followed by hurdles in its conventional diagnosis and treatment. The characteristic mechanism of nanoparticles for efficiently tracing brain tumour grade and delivery of therapeutic genes or drugs has been summarised. Nanocarriers like liposomes have been widely used and commercialized for human brain cancer treatment. However, nano-inspired structures await their translational recognition. The green synthesis of nanomaterials and their advantages have been discussed. The article highlights the challenges in the nano-modulation of brain cancer and its future outlook.