AbstractHeterostructured transition metal dichalcogenides (TMDs) have received much attention due to their tunable optical and electronic properties. Here, a strategy for facile fabrication of porous anodic alumina (PAA) membrane‐supported monolayer molybdenum disulfide (MoS2) is described. PAA is either empty or filled with gold nanoparticles (AuNPs). Such nanopore/nanosphere‐supported MoS2 (i.e., PAA‐MoS2 and PAA‐Au‐MoS2) exhibits greatly enhanced optical performances compared with those of silicon wafer‐supported MoS2 (i.e., Si/SiO2‐MoS2). Notably, 11‐fold Raman enhancement, 13‐fold photoluminescence enhancement, and 419‐fold second‐harmonic generation enhancement are achieved in PAA‐Au‐MoS2. Moreover, the optical enhancement mechanism of this unique structure is proposed. This work provides a platform for the construction of curved/heterostructured TMDs and exploration of their strong light‐matter interactions.