Nickel(II)–salen or nickel(II)–salphen catalyzed α-alkylation of ketones and nitriles with primary alcohols is reported. Various α-alkylated ketones and nitriles were obtained in high yields through a borrowing hydrogen strategy by using 1–3 mol% of nickel catalyst and a catalytic amount of NaOH (5–10 mol%) under aerobic conditions.