The present invention discloses a rare-earth-manganese/cerium-zirconium-based composite compound, a method for preparing the same, and a use thereof. The composite compound is of a core-shell structure with a general formula expressed as: A REcBaOb-(1-A)CexZr(1-x-y)MyO2-z, wherein 0.1≤A≤0.3, preferably 0.1≤A≤0.2; a shell layer has a main component of rare-earth manganese oxide with a general formula of REcMnaOb, wherein RE is a rare-earth element or a combination of more than one rare-earth elements, and B is Mn or a combination of Mn and a transition metal element, 1≤a≤8, 2≤b≤18, and 0.25≤c≤4; and a core has a main component of cerium-zirconium composite oxide with a general formula of CexZr(1-x-y)MyO2-z, wherein M is one or more non-cerium rare-earth elements, 0.1≤x≤0.9, 0≤y≤0.3, and 0.01≤z≤0.3. The composite compound enhances an oxygen storage capacity of a cerium-zirconium material through an interface effect, thereby increasing a conversion rate of a nitrogen oxide.