We report a new strategy for ligand-free attachment of plasmonic Au nanoparticles on the surface of a ZnO nanowire to make high-performance broadband photodetectors using a pulsed laser ablation technique in a liquid medium. The photoresponse of the ZnO-based photodetector is enhanced and the photodetection limit is broadened from UV to visible, which can be controlled by varying the concentration of Au nanoparticles attached to the ZnO surface. This Au nanoparticle concentration can be tuned by varying the number of laser pulses used in the ablation process. We found that the responsivity of the detector is 10 mA W for [Formula: see text] and increases to as much as 0.4 A W for λ ≤ 400 nm for the maximum Au concentration. The enhanced responsivity was found to be linked to increased absorption over a broad spectral range arising from direct and indirect plasmonic processes due to Au nanoparticle attachment, and the enhanced absorption also leads to a large increment in photocurrent generation. We also found that the attachment of Au nanoparticles makes the relaxation of the photocurrent (persistence) considerably faster in both the UV and visible regions of the spectrum and that the persistence directly depends on the concentration of Au nanoparticles attached to the ZnO nanowire. This single-step pulsed laser ablation-based nanoparticle attachment process can be further used to make other plasmonic nanoparticle-decorated nanowire devices.