Carbonaceous nanomaterials (CNMs) have drawn tremendous biomedical research interest because of their unique structural features. Recently, CNMs, namely carbon dots, fullerenes, graphene, etc, have been successful in establishing them as considerable nanotherapeutics for phototherapy applications due to their electrical, thermal, and surface properties. This review aims to crosstalk the current understanding of CNMs as multimodal compounds in photothermal and photodynamic therapies as an integrated approach to treating cancer. It also expounds on phototherapy’s biomechanics and illustrates its relation to cancer biomodulation. Critical considerations related to the structural properties, fabrication approaches, surface functionalization strategies, and biosafety profiles of CNMs have been explained. This article provides an overview of the most recent developments in the study of CNMs used in phototherapy, emphasizing their usage as nanocarriers. To conquer the current challenges of CNMs, we can raise the standard of cancer therapy for patients. The review will be of interest to the researchers working in the area of photothermal and photodynamic therapies and aiming to explore CNMs and their conjugates in cancer therapy.