Advances in nanomaterials science contributed in recent years to develop new devices and systems in the micro and nanoscale for improving the diagnosis and treatment of cancer. Substantial evidences associate cancer cells and tumor microenvironment with reactive oxygen species (ROS), while conventional cancer treatments and particularly radiotherapy, are often mediated by ROS increase. However, the poor selectivity and the toxicity of these therapies encourage researchers to focus efforts in order to enhance delivery and to decrease side effects. Thus, the development of redox-active nanomaterials is an interesting approach to improve selectivity and outcome of cancer treatments. Herein, we describe an overview of recent advances in redox nanomaterials in the context of current and emerging strategies for cancer therapy based on ROS modulation.