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Abstract The precise deployment of functional payloads to plant tissues is a new approach to help advance the fundamental understanding of plant biology and accelerate plant engineering. Here, the design of a silk‐based biomaterial is reported to fabricate a microneedle‐like device, dubbed “phytoinjector,” capable of delivering a variety of payloads ranging from small molecules to large proteins into specific loci of various plant tissues. It is shown that phytoinjector can be used to deliver payloads into plant vasculature to study material transport in xylem and phloem and to perform complex biochemical reactions in situ. In another application, it is demonstratedAgrobacterium‐mediated gene transfer to shoot apical meristem (SAM) and leaves at various stages of growth. Tuning of the material composition enables the fabrication of another device, dubbed “phytosampler,” which is used to precisely sample plant sap. The design of plant‐specific biomaterials to fabricate devices for drug deliveryin plantaopens new avenues to enhance plant resistance to biotic and abiotic stresses, provides new tools for diagnostics, and enables new opportunities in plant engineering.