A versatile, solution‐processed fabrication strategy combining interference lithography, electroplating, and imprint transfer is developed to realize plastic plasmonic metasurfaces for biomolecular sensing applications. This process is potentially suitable for high‐throughput, large‐volume, and low‐cost production of plasmonic metasurfaces. Gold nanocheckerboard metasurfaces are fabricated using this method and show enhanced performance in plasmonic refractometric sensing applications compared to other localized surface plasmon resonance (LSPR) sensors. An excellent refractive index sensitivity of 435.1 nm RIU−1 and a figure of merit (FoM) of 7.38 are demonstrated for the prototype plasmonic sensors at wavelengths of 570–610 nm. The spectral regions used in sensing are located within the operating wavelength of silicon photodiodes, which allows low analytical instrumentation cost. A plasmonic biosensor is also constructed on the metasurfaces by monitoring the LSPR peak shift that occurs upon high‐affinity biomolecular interactions between bovine serum albumin (BSA) and anti‐BSA proteins. Moreover, excellent mechanical stability against repeated bending is demonstrated for the plasmonic sensor, which is essential for wearable sensing devices.

Metasurfaces with metallic [1] and dielectric [2] nanophotonic building blocks manipulate light scattering in the subwavelength

With the growing importance of three-dimensional (3D) nanomaterials and devices, there has been a great demand for highfidelity, full profile topographic characterizations in a nondestructive manner. A promising route is to employ a high-aspect-ratio (HAR) probe in atomic force microscopy (AFM) imaging. However, the fabrication of HAR-AFM probes continues to suffer from extravagant cost, limited material choice, and complicated manufacturing steps. Here, we report one-step, on-demand electrohydrodynamic 3D printing of metallic HAR-AFM probes with tailored dimensions. Our additive fabrication approach yields a freestanding metallic nanowire with an aspect ratio over 30 directly on a cantilever within tens of seconds, producing a HAR-AFM probe. Furthermore, the benefits associated with unprecedented simplicity in the probe's dimension control, material selection, and regeneration are provided. The 3D-printed HAR-AFM probe exhibits a better fidelity in deep trench AFM imaging than a standard pyramidal probe. We expect this approach to find facile, material-saving manufacturing routes in particular for customizing functional nanoprobes.