Plasmonic superlattice membrane exhibits remarkable functional properties that are emerging from engineered assemblies of well-defined "meta-atoms," which is featured as a conceptual new category of two-dimensional optical metamaterials. The ability to build plasmonic membranes over macroscopic surfaces but with nanoscale ordering is crucial for systematically controlling the light-matter interactions and represents considerable advances for the bottom-up fabrication of soft optoelectronic devices and circuits. Through rational design, novel nanocrystals, and by engineering the packing orders, the hybridized plasmon signature can be customized, promoting controllable near-field confinement for surface-enhanced Raman scattering (SERS) based detection. However, building such 2D architectures has proven to be remarkably challenging due to the complicated interparticle forces and multiscale interactions during self-assembly. Here, we report on the fabrication of ultralong-nanobrick-based giant plasmonic superlattice membranes as high-performance SERS substrates for ultrasensitive and label-free protein detection. Using aspect-ratio controllable short-to-ultralong nanobricks as building blocks, we construct three distinctive plasmonic membranes by polymer-ligand-based strategy in drying-mediated self-assembly at the air/water interfaces. The plasmonic membranes exhibit monolayered morphology with nanoscale assembled ordering but macroscopic lateral dimensions, inducing enhanced near-field confinement and uniform hot-spot distribution. By choosing 4-aminothiophenol and bovine serum albumin (BSA) as a model analyte, we establish an ultrasensitive assay for label-free SERS detection. The detection limit of BSA can reach 15 nM, and the enhancement factor reached 4.3 × 105, enabling a promising avenue for its clinical application in ultrasensitive biodiagnostics.