The undesirable side effects of conventional chemotherapy are one of the major problems associated with cancer treatment. Recently, with the development of novel nanomaterials, tumor-targeted therapies have been invented in order to achieve more specific cancer treatment with reduced unfavorable side effects of chemotherapic agents on human cells. However, the clinical application of nanomedicines has some shortages, such as the reduced ability to cross biological barriers and undesirable side effects in normal cells. In this order, bioinspired materials are developed to minimize the related side effects due to their excellent biocompatibility and higher accumulation therapies. As bioinspired and biomimetic materials are mainly composed of a nanometric functional agent and a biologic component, they can possess both the physicochemical properties of nanomaterials and the advantages of biologic agents, such as prolonged circulation time, enhanced biocompatibility, immune modulation, and specific targeting for cancerous cells. Among the nanomaterials, asymmetric nanomaterials have gained attention as they provide a larger surface area with more active functional sites compared to symmetric nanomaterials. Additionally, the asymmetric nanomaterials are able to function as two or more distinct components due to their asymmetric structure. The mentioned properties result in unique physiochemical properties of asymmetric nanomaterials, which makes them desirable materials for anti-cancer drug delivery systems or cancer bio-imaging systems. In this review, we discuss the use of bioinspired and biomimetic materials in the treatment of cancer, with a special focus on asymmetric nanoparticle anti-cancer agents.