Combining a two-dimensional (2D) morphology and plasmonic photocatalysis represents an efficient design for light-driven organic transformations. We report a one-pot synthesis of surfactant templated PdAu nanosheets (NSs). Transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) analyses show the formation of 2D PdAu structures was initiated through nanoparticle seeds dispersed in the alkyl ammonium salt surfactant which acted as a template for the growth into NSs. The PdAu NSs were used for visible-light-enhanced Suzuki cross coupling. The PdAu bimetallic NSs outperformed monometallic Pd NSs and commercial Pd/C in room-temperature Suzuki cross-coupling reactions. The high catalytic activity is attributed to a combination of the 2D morphology giving rise to plasmon-enhanced catalysis and a high density of surface atoms, the electron-rich Pd surface due to alloying, and the presence of weakly bound amines. A comparative study of surfactant-assisted NSs and CO-assisted NSs was also carried out to assess the influence of surface ligands on the catalytic and photocatalytic enhancement of NSs with similar morphology. The surfactant-assisted NSs showed substantially superior performance compared to the CO-assisted for room-temperature Suzuki coupling reactions.