AbstractThe versatility of nanodiamonds (NDs) as a polymer‐embedded therapeutic vehicle was demonstrated by the development of a hybrid material consisting of a poly(ethylene glycol) diacrylate (PEGDA) hydrogel embedded with ND‐drug complexes. A wide range of PEGDA structures, including single and multiple drug reservoirs, exhibited high loading capabilities and stable slow‐release, augmented with the addition of ND conjugates. ND‐PEGDA hydrogels were compared to unmodified, drug‐embedded PEGDA hydrogels to demonstrate their robust drug sequestering capacity in vitro. Remarkably, ND‐embedded hydrogels were capable of mitigating the harmful effects of burst‐release by displaying slow and controlled administration of therapeutic compounds, an improvement over standard diffusion‐based release profiles. The tunable customization of PEGDA hydrogel, both in structure and content, as well as its facile methods of synthesis, make this material an effective multi‐therapeutic complement to the drug delivery abilities of NDs. A hybrid material that utilizes the synergy of PEGDA and ND components has the potential for applications toward a diverse array of biomedical challenges. magnified imageAn artistic rendering of a multi‐layered PEGDA patch. The center of the patch (purple) contains drug‐bound ND particles that are being released (gray truncated octahedra with purple glow), while the outer ring depicts the molecule Temozolomide (green). This image illustrates the ability for tiered patches to simultaneously administer multiple drugs, as well as the drug‐sequestering ability of NDs that mediates sustained delivery and reduced burst release. The nested structure of the two drugs was designed so that the therapeutics could be released sequentially, at different peak‐elution time intervals.