Plasmonic nanostructures, which exhibit notable localized surface plasmon resonance (LSPR) properties, are a promising approach for improving the efficiency of fiber‐shaped dye‐sensitized solar cells (FDSSCs) and flexible organic light‐emitting diodes (FOLEDs). Herein, novel plasmonic nanostructure is successfully synthesized via the self‐densification of gold nanoparticles (Au NPs) onto a genetically engineered M13 bacteriophage template. The synthesized Au NP‐M13 bio‐nanostructure show extraordinary gap‐plasmon effects and significantly enhanced LSPR properties compared to randomly dispersed Au NPs for both solid‐state FDSSCs (SS‐FDSSCs) and FOLEDs. Briefly, a power conversion efficiency (PCE) increment of 40.7% is recorded for the Au metallic NPs‐anchored M13 bacteriophage (Au NPs‐M13) enhanced SS‐FDSSCs; whereas an external quantum efficiency (EQE) increment of 47.2% is achieved for the Au NPs‐M13 enhanced FOLEDs.