Introduction: Current brain cancer treatments, based on radiotherapy and chemotherapy, are sometimes successful, but they are not free of drawbacks. Areas covered: Traditional methods for the treatment of brain tumors are discussed here with new solutions presented, among which the application of nanotechnology has demonstrated promising results over the past decade. The traditional synthesis of nanostructures, which relies on the use of physicochemical methodologies are discussed, and their associated concerns in terms of environmental and health impact due to the production of toxic by-products, need for toxic catalysts, and their lack of biocompatibility are presented. An overview of the current situation for treating brain tumors using nanotechnological-based approaches is introduced, and some of the latest advances in the application of green nanomaterials (NMs) for the effective targeting of brain tumors are presented. Expert opinion: Green nanotechnology is introduced as a potential solution to toxic NMs through the application of environmentally friendly and cost-effective protocols using living organisms and biomolecules. The current status of this field, such as those involving clinical trials, is included, and the possible limitations of green-NMs and potential ways to avoid those limitations are discussed so that the field can potentially evolve.