It is always highly pursued to develop efficient and durable catalysts for catalytic applications. Herein, intermetallic PdBi aerogels with tunable activity were prepared successfully via a surfactant-free spontaneous gelation process. The prepared PdBi aerogels have a three-dimensional high porous structure and plentiful active sites pervaded on the ultrathin interlinked nanowires network. These unique structures, as well as the synergistic effect between Pd and Bi, can accelerate mass and electron transfer, and improve the atom utilization ratio of Pd atoms to promote the catalytic efficiency. As a proof-of-concept application, the optimized Pd2Bi1 aerogels exhibit 4.2 and 6.2 times higher catalytic activity for the reduction of 4-nitrophenol (4-NP) and methylene blue (MB) than those of commercial Pd/C, respectively. With the introduction of non-noble metal of Bi, the cost of the resulted PdBi aerogels can be dropped significantly while the catalytic capability of PdBi aerogel will be improved sharply. This strategy will bring good hints to rationally design fine catalysts for various applications.