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Herein, multifunctional mimics of viral architectures and infections self-assembled from tailor-made dendritic lipopeptides for programmed targeted drug delivery are reported. These viral mimics not only have virus-like components and nanostructures, but also possess virus-like infections to solid tumor and tumor cells. Encouragingly, the viral mimics provide the following distinguished features for tumor-specific systemic delivery: i) stealthy surface to resist protein interactions and prolong circulation time in blood, ii) well-defined nanostructure for passive targeting to solid tumor site, iii) charge-tunable shielding for tumor extracellular pH targeting, iv) receptor-mediated targeting to enhance tumor-specific uptake, and v) supramolecular lysine-rich architectures mimicking viral subcellular targeting for efficient endosomal escape and nuclear delivery. This bioinspired design make in vivo tumor suppression by drug-loaded viral mimics against BALB/c mice bearing 4T1 tumor greatly exceed the positive control group (more than three times). More importantly, viral mimics hold great potentials to reduce side effects and decrease tumor metastasis after systemic administration. [ABSTRACT FROM AUTHOR]

X. Xu, Z. Gu, and co‐workers show on page 5250 that dendritic lipopeptide‐based mimics of viral architectures can serve as a versatile nanoplatform for tumor‐targeted drug delivery. The receptor‐mediated targeting and subcellular targeting can greatly promote therapeutic index of antitumor drugs, reducing side effects and decreasing tumor metastasis after systemic administration. [ABSTRACT FROM AUTHOR]