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The area of molecular magnetic coolants has developed rapidly in recent years. A large number of competitive candidates have been reported, with the cooling performances chasing each other. In this account, four explicit strategies, namely, increasing ground-state spin, reducing magnetic anisotropy, weakening magnetic interactions, and lowering the molecular weight, are proposed from the theoretical viewpoint towards improving the magnetocaloric effect (MCE). According to this guidance, these successful strategies are discussed to pursue excellent magnetic coolants. This is accompanied by a discussion of the representative examples reported by our group. The magnetic entropy change increases from one compound to another, which in the most pronounced cases is suggestive of being the largest MCE in magnetic coolants. [ABSTRACT FROM AUTHOR]