Gold-based catalysts occupy one of the largest segments in catalysis science and technology. (Ultra)small Au nanoparticles (<5 nm) show exceptional catalytic activity in a number of homogeneous and heterogeneous reactions. The performance can be further intensified by applying advanced preparation techniques that ensure predesigned surface and morphological features. Pulsed laser ablation in gas or liquid is a promising approach that allows producing various pristine and supported mono- and bimetallic Au-based materials (high-entropy materials, single-atom species, etc.) with unique catalytic and plasmonic properties. This review is focused on the preparation using pulsed laser ablation and the application of Au-based catalytically active materials. The recent publications for the last 5 years are analyzed with special attention being paid to synthesis-structure-performance relationships. These aspects are considered in photo- and electrocatalytic applications, reduction of CO2 and N containing compounds, including nitroaromatics, organic dyes, and inorganic complexes.