An uncoordinated salen-containing metal-organic framework (MOF) obtained through postsynthesis removal of Mn(III) ions from a metallosalen-containing MOF material has been used for selective separation of Th(IV) ion from Ln(III) ions in methanol solutions for the first time. This material exhibited an adsorption capacity of 46.345 mg of Th/g. The separation factors (beta) of Th(IV)/La(III), Th(IV)/Eu(III), and Th(IV)/Lu(III) were 10.7, 16.4, and 10.3, respectively.