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New carbon–carbon bond formation reactions expand our horizon of retrosynthetic analysis for the synthesis of complex organic molecules. Although many methods are now available for the formation of C(sp²)–C(sp³) and C(sp³)–C(sp³) bonds via transition metal-catalyzed cross-coupling of alkyl organometallic reagents, direct use of readily available olefins in a formal fashion of hydrocarbonation to make C(sp²)–C(sp³) and C(sp³)–C(sp³) bonds remains to be developed. Here we report the discovery of a general process for the intermolecular reductive coupling of unactivated olefins with alkyl or aryl electrophiles under the promotion of a simple nickel catalyst system. This new reaction presents a conceptually unique and practical strategy for the construction of C(sp²)–C(sp³) and C(sp³)–C(sp³) bonds without using any organometallic reagent. The reductive olefin hydrocarbonation also exhibits excellent …