Nanomaterials that can be assembled with a high degree of control over their physical features are of interest for use in a variety of biological and therapeutic applications. Biotemplated nanomaterials have demonstrated great promise in this regard, owing to their ability to overcome low solubility, off-target toxicity, and poor biodegradability. There remains an important unmet need: trackable nanomaterials that are also highly biocompatible. Ideally, these would also be readily synthesized in a controllable manner.
Here, we report self-assembled quantum dot DNA hydrogels (QDH) that exhibit both size and spectral tunability. We successfully incorporate DNA-templated quantum dots with high quantum yield, long-term photostability, and low cytotoxicity into a hydrogel network in a single step. By leveraging DNA-guided interactions, we introduce multifunctionality for a variety of applications, including enzyme-responsive drug delivery and cell-specific targeting. We report that QDH delivery of doxorubicin, an anticancer drug, therapeutic efficacy in in vivo increases potency 9-fold against cancer cells. This approach also demonstrated high biocompatibility, trackability, and breastcancer xenograft mice. This work paves the way for the development of newtunable biotemplated nanomaterials with multiple synergistic functionalities for biomedical applications.