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Organic compounds, composed of carbon, hydrogen, and a few additional heteroatoms, represent highly diverse and attractive substances. They play crucial roles in our daily lives, serving as polymers, organic electronic materials, pharmaceuticals, and so on. Most of them are synthesized by humans, primarily derived from petroleum. Organic synthetic chemistry is the foundational science to study efficient methods to construct diverse organic molecules with minimal waste. In my Hakubi research project, I focus on developing novel catalysts to activate non-reactive carbon–hydrogen bonds prevalent in organic compound backbones. While such reactions, so-called C–H activation, have been extensively studied all over the world, my emphasis lies in developing reactions that are genuinely synthetically useful and applicable to practical industrial production in the future. I tackle this challenging task through both experimental and computational chemistry.