Graphene‐based materials have shown immense pertinence for sensing/imaging, gene/drug delivery, cancer therapy/diagnosis, and tissue engineering/regenerative medicine. Indeed, the large surface area, ease of functionalization, high drug loading capacity, and reactive oxygen species induction potentials have rendered graphene‐ (G‐) and graphene oxide (GO)‐based (nano)structures promising candidates for cancer therapy applications. Various techniques namely liquid‐phase exfoliation, Hummer's method, chemical vapor deposition, chemically reduced GO, mechanical cleavage of graphite, arc discharge of graphite, and thermal fusion have been deployed for the production of G‐based materials. Additionally, important criteria such as biocompatibility, bio‐toxicity, dispersibility, immunological compatibility, and inflammatory reactions of G‐based structures need to be systematically assessed for additional clinical and biomedical appliances. Furthermore, surface properties (e.g., lateral dimension, charge, corona influence, surface structure, and oxygen content), concentration, detection strategies, and cell types are vital for anticancer activities of these structures. Notably, the efficient accumulation of anticancer drugs in tumor targets/tissues, controlled cellular uptake properties, tumor‐targeted drug release behavior, and selective toxicity toward the cells are crucial criteria that need to be met for developing future anticancer G‐based nanosystems. Herein, important challenges and future perspectives of cancer therapy using G‐ and GO‐based nanosystems have been highlighted, and the recent advancements are deliberated.