The selective functionalization of C–H bonds is a critical step in the majority of synthetic organic pathways. Our research lab, among others, takes inspiration from the reactivity of Cu-dependent metalloenzymes to design catalytic systems for the C–H oxidation of challenging substrates (i.e., alkanes). In this Synpacts article, we summarize our recent findings on the Cu-catalyzed peroxidation of C–H bonds with H2O2 under mild conditions.