Early medical diagnostic in nanomedicine requires the implementation of innovative nanosensors with highly sensitive, selective, and reliable biomarker detection abilities. In this paper, a dual Localized Surface Plasmon Resonance - Surface Enhanced Raman Scattering (LSPR- SERS) immunosensor based on a flexible three-dimensional (3D) gold (Au) nanocups platform has been implemented for the first time to operate as a relevant "proof-of-concept" for the specific detection of antigen-antibody binding events, using the human IgG - anti-human IgG recognition interaction as a model. Specifically, polydimethylsilane (PDMS) elastomer mold coated with a thin Au film employed for pattern replication of hexagonally close-packed monolayer of polystyrene nanospheres configuration has been employed as plasmonic nanoplatform to convey both SERS and LSPR readout signals, exhibiting both well-defined LSPR response and enhanced 3D electromagnetic field. Synergistic LSPR and SERS sensing use the same reproducible and large-area plasmonic nanoplatform providing complimentary information not only on the presence of anti-human IgG (by LSPR) but also to identify its specific molecular signature by SERS. The development of such smart flexible healthcare nanosensor platforms holds promise for mass production, opening thereby the doors for the next generation of portable point-of-care devices.