This paper presents for the first time a programmable and scalable 3D electro-bioprinting (3D-EBP) process for patterning bionanoreceptors, cysteine-modified Tobacco mosaic virus (TMV1cys), on high-density micropillar array electrodes. The structural hydrophobicity in high aspect ratio geometries of micro/nano devices poses a critical challenge for assembling 3D biomaterial-device interfaces. Here, we have successfully integrated electrowetting principles with a modified state-of-the-art bioprinter for automated, high-throughput, and large-scale patterning of TMV1cys particles on hydrophobic 3D electrodes. The 3D-EBP processed bionanoreceptors maintained both structural and chemical functions as characterized via SEM and fluorescence microscopy. Overall, the innovative 3D biomanufacturing process creates excellent opportunities for advancing on-demand biointegrated devices including multiplexed biosensors and bioenergy harvesting devices.