Simple Peptide-Tuned Self-Assembly of Photosensitizers towards Anticancer Photodynamic Therapy

Peptide‐tuned self‐assembly of functional components offers a strategy towards improved properties and unique functions of materials, but the requirement of many different functions and a lack of understanding of complex structures present a high barrier for applications. Herein, we report a photosensitive drug delivery system for photodynamic therapy (PDT) by a simple dipeptide‐ or amphiphilic amino‐acid‐tuned self‐assembly of photosensitizers (PSs). The assembled nanodrugs exhibit multiple favorable therapeutic features, including tunable size, high loading efficiency, and on‐demand drug release responding to pH, surfactant, and enzyme stimuli, as well as preferable cellular uptake and biodistribution. These features result in greatly enhanced PDT efficacy in vitro and in vivo, leading to almost complete tumor eradication in mice receiving a single drug dose and a single exposure to light. Simple but effective: Amphiphilic dipeptides or amino acids can tune the self‐assembly of photosensitizers (PS) towards anticancer photodynamic therapy. Simple components to realize the nanofabrication of therapeutic agents based on cooperative self‐assembly represent a versatile and robust approach towards anticancer therapy.