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A novel property is that a cocommutative post-Hopf algebra gives rise to a generalized Grossman-Larson product, which leads to a subadjacent Hopf algebra and can be used to construct solutions to the Yang-Baxter equation. Then, we introduce the notion of relative Rota-Baxter operator on Hopf algebras. A cocommutative post-Hopf algebra gives rise to a relative Rota-Baxter operator on its subadjacent Hopf algebra. Conversely, a relative Rota-Baxter operator also induces a post-Hopf algebra. Finally, we show that relative Rota-Baxter operators give rise to matched pairs of Hopf algebras. 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