Supramolecular biomaterials exploit rationally-designed non-covalent interactions to enable innovative approaches to drug formulation and delivery. For example, supramolecular interactions can be used to dynamically cross-linking polymer networks, yielding shear-thinning and self-healing hydrogels that allow for minimally invasive implantation in vivo though direct injection or catheter delivery to tissues. Herein, we discuss the preparation and application of shear-thinning, injectable hydrogels driven by non-covalent interactions between modified biopolymers (BPs) and biodegradable nanoparticles (NPs) comprised of poly(ethylene glycol)-block-poly(lactic acid) (PEG-b-PLA). Owing to the non-covalent interactions between PEG-b-PLA NPs and BPs, the hydrogels flow under applied stress and their mechanical properties recover completely within seconds when the stress is relaxed, demonstrating the shear-thinning and injectable nature of the material. The hierarchical construction of these biphasic hydrogels allows for multiple therapeutic compounds to be entrapped simultaneously and delivered with identical release profiles, regardless of their chemical make-up, over user-defined timeframes ranging from days to months. These materials enable novel approaches to immunotherapy, which rely on precise release of complex mixtures of compounds, as well as long-term treatment strategies for a variety of disease targets. Overall, this presentation will demonstrate the utility of a supramolecular approach to the design of biomaterials affording unique opportunities in the formulation and controlled release of therapeutics.