| Summary: | Abstract Clinical trials have generated encouraging outcomes for the utility of thermal agents (TAs) in cancer thermal therapy (TT). Although the fast breakdown of TAs alleviates safety concerns, it restricts the thermal stability necessary for effective treatment. TAs with excellent thermal stability, on the other hand, deteriorate slowly. Rare are the approaches that address the trade-off between high thermal stability and quick deterioration of TAs. Here we control the thermal signature of WS2-type 2D materials by utilizing previously undescribed DOX–WS2–PEG–M13 nanostructures (we term them D nanostructures) through Joule heating phenomena, and develop an integrated system for TT for enhancing thermal performance, and simultaneously, maintaining rapid degradation, and chemotherapy for efficacious treatment. A relative cell viability of ~ 50% was achieved by the D-based TT (DTT) configuration, as well as a 1 nM drug concentration. The D-driven chemotherapy (DCT) model also attains a relative cell viability of 80% for 1 nM drug concentration, while a 1-week degradation time was revealed by the D nanostructure. Theoretical studies elucidate the drug molecule–nanostructure and drug-on-nanostructure–solution interaction-facilitated enhancement in drug loading and drug release performance in DCT varieties. As a result, this work not only proposes a “ideal TA” that circumvents TA restrictions, but also enables proof-of-concept application of WS2-based materials in chemotherapy-unified combination cancer therapy. Graphical Abstract
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