Heterometallic nanoparticles (NPs) have been emerging as a type of important catalyst. Bimetallic NPs with alloyed and core–shell structures have higher activities than monometallic counterparts in catalysis due to the synergistic effects between the two metals. Compared to the straightforward synthesis of bimetallic alloy NPs, the preparation strategies for bimetallic core–shell NPs are flexible and diversified. In addition, synergistic catalysis over trimetallic and multimetallic NPs has also received considerable interest in recent years. In this feature article, we provide an overview of the recent developments of heterometallic NPs for improved catalytic performance.