Learning from nature is a powerful and effective means to design synthetic building blocks for creation of entirely novel materials. Synthetic peptide building blocks inspired by nature are more versatile and flexible for this purpose due to their controllable constituents, tailorable functions and ease of availability. Hence, peptide based supramolecular materials have shown numerous advantages in biomedical applications. However, in the area of tumor therapy, the assembled peptide materials usually are only applied as drug delivery vehicles for delivering of anti-tumor drugs, which usually have a low loading capability and ignore the merits of controllable self-assembly, and thus, suffer from the limited therapeutic and undesired side effects of the drugs. One promising strategy which is rarely studied is the controlled assembly of peptide-drug conjugates toward enhanced antitumor therapeutic efficiency and lowered negative side effects. Through such a strategy, a high drug loading capability can be readily achieved and the delivery of drugs can be manipulated by controlling the supramolecular properties of the formed nanostructures. In this project research consortia proposes novel molecular design, synthesis, self-assembly, and potential applications of peptide-photosensitizer conjugates in photodynamic therapy (PDT) against cancers.