Dual-Targeting Multivalent Aptamer-Drug Hybrids for Synergistic Cancer Immunotherapy

J Am Chem Soc. 2026 Apr 22;148(15):15782-15796. doi: 10.1021/jacs.5c21968. Epub 2026 Apr 13.

Abstract

Targeted drug conjugates (TDCs) have transformed cancer therapy by enabling selective delivery of cytotoxic agents, yet most existing designs rely on single-antigen targeting and single-payload architectures that limit efficacy in heterogeneous tumors and restrict opportunities for integrating orthogonal mechanisms of action. Here, we report circular, dual-targeting multivalent aptamer-drug hybrids (Dualo-mvApDHsD/S) that codeliver doxorubicin (Dox) and STING agonist (diABZI) for synergistic chemo-immunotherapy. Built on a programmable DNA scaffold with defined valence and high loading capacity, the Dualo-mvApDHsD/S simultaneously engage c-Met and CD71 to enhance tumor-specific uptake through heteromultireceptor-mediated endocytosis, achieving efficient intracellular delivery and robust tumor accumulation in vivo. Within tumor cells, Dox induces genotoxic stress and potent immunogenic cell death, while diABZI activates cGAS-STING signaling to amplify type I interferon responses. This coordinated action remodels the immunosuppressive tumor microenvironment, promoting dendritic cell recruitment and activation, expanding IFN-responsive macrophages and conventional dendritic cells, and driving the proliferation and functional maintenance of cytotoxic CD8+ T cells. Single-cell RNA and TCR sequencing revealed increased TCR diversity, reduced terminal exhaustion, and strengthened effector differentiation in response to combination therapy. Notably, Dualo-mvApDHsD/S synergize with PD-1 blockade to achieve durable tumor eradication and long-term protection. These findings establish multivalent aptamer-drug hybrids as a versatile platform for multitarget, multipayload precision therapeutics and highlight their potential for next-generation TDC design.

MeSH terms

  • Animals
  • Antineoplastic Agents* / chemistry
  • Antineoplastic Agents* / pharmacology
  • Aptamers, Nucleotide* / chemistry
  • Aptamers, Nucleotide* / pharmacology
  • Cell Line, Tumor
  • Doxorubicin* / chemistry
  • Doxorubicin* / pharmacology
  • Doxorubicin* / therapeutic use
  • Humans
  • Immunotherapy*
  • Membrane Proteins / agonists
  • Mice
  • Neoplasms* / drug therapy
  • Neoplasms* / therapy

Substances

  • Aptamers, Nucleotide
  • Doxorubicin
  • Antineoplastic Agents
  • Membrane Proteins