This account is to commemorate the retirement of Jean-Marie Basset from the KAUST Catalysis Center after a career spanning almost five decades. Jean-Marie has been a leading figure in the world of heterogeneous catalysis. Rather than studying supported catalysts through the traditional lens of surface science, he brought an approach of molecular organometallic chemistry to the field. In the process, Jean-Marie established the field of surface organometallic chemistry. During the first phase of his career, he pioneered ways to synthesize and characterize well-defined metal sites on oxide and metal surfaces. Through this work, the Basset group could establish structure–activity relationships on supported catalyst materials and also show that the rules known to govern the catalytic cycles of homogeneous catalysts could be employed to understand and enhance heterogeneous catalyst reactions. From this key insight, Jean-Marie developed the concept of heterogeneous catalysis by design, synthesizing surface organometallic fragments that were thought to form a part of the catalytic cycle. From this standpoint, the Basset group has improved the activity, selectivity, and sustainability of numerous known reactions and also discovered multiple reactions, including the Ziegler–Natta depolymerization, the metathesis of alkanes, the coupling of methane to ethane and hydrogen, the cleavage of alkanes by methane, the metathesis of imines, the metathetic cleavage of olefins to aldehydes by molecular oxygen, and the hydro-metathesis of olefins.