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Transition-metal-catalyzed C–H activation has emerged as a powerful strategy for molecular synthesis with unique levels of resource economy. Weak secondary dispersion interactions were found to play an essential role in these transformations in terms of kinetic efficacy and selectivity. This Account summarizes our group's recent progress in the rationalization and quantification of London dispersion effects within the transition-metal-catalyzed C–H activation. 1 Introduction 2 Annulation Reactions 3 Alkylation Reactions 4 Arylation Reactions 5 Olefination Reactions 6 Oxygenation Reactions 7 Conclusion [ABSTRACT FROM AUTHOR]