Anisotropic 2D materials with unique thermoelectric, electrical, and optical characteristics offer prospects for various angle-dependent devices. Yet, few anisotropic 2D materials are exploited. Black phosphorus (BP) is a newly rediscovered 2D material with striking in-plane anisotropy. However, experimental illustrations of the optical anisotropy of 2D BP are very limited presumably due to the ultrathin thickness of the few-layered BP which weakens the lightmatter interaction. To solve this problem, herein a hybrid nanostructure is fabricated using a one-step self-assembly deposition of gold (Au) nanoparticle (NP) clusters onto the few-layered BP residing on a silica (SiO 2) substrate. Such a hybrid nanostructure can squeeze the light into AuNPs-SiO 2 gap through the gap plasmon resonance, enabling the confined light to interact efficiently with the ultrathin BP film. Angle-resolved polarized Raman spectra measurement is carried out to study the influence of the AuNPs on the in-plane optical anisotropy of the BP. About 20 times enhancement of Raman intensity anisotropy is experimentally achieved using AuNPs. The AuNPs-BP system is not only useful for high-performance polarization-dependent photonic devices but also a universal methodology for exploring the in-plane anisotropy of low-symmetry 2D materials. Furthermore, the high-throughput self-assembly fabrication shows its potential for industrial-scale manufacturability.