The application of nanomaterials (NMs) in biomedicine is increasing rapidly and offers excellent prospects for the development of new non-invasive strategies for the diagnosis and treatment of cancer. In this review, we provide a brief description of cancer pathology and the characteristics that are important for tumor-targeted NM design, followed by an overview of the different types of NMs explored to date, covering synthetic aspects and approaches explored for their application in unimodal and multimodal imaging, diagnosis and therapy. Significant synthetic advances now allow for the preparation of NMs with highly controlled geometry, surface charge, physicochemical properties, and the decoration of their surfaces with polymers and bioactive molecules in order to improve biocompatibility and to achieve active targeting. This is stimulating the development of a diverse range of nanometer-sized objects that can recognize cancer tissue, enabling visualization of tumors, delivery of anti-cancer drugs and/or the destruction of tumors by different therapeutic techniques.