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Herein, we report a manganese‐catalyzed three‐component coupling of secondary alcohols, primary alcohols and methanol for the synthesis of β,β‐methylated/alkylated secondary alcohols. Using our method, a series of 1‐arylethanol, benzyl alcohol derivatives, and methanol undergo sequential coupling efficiently to construct assembled alcohols with high chemoselectivity in moderate to good yields. Mechanistic studies suggest that the reaction proceeds via methylation of a benzylated secondary alcohol intermediate to generate the final product. [ABSTRACT FROM AUTHOR]