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An initial data set \\((M,g)\\) is a connected complete Riemannian \\(3\\)-manifold such that there exists a bounded open set \\(U\\subset M\\) with \\(M\\setminus U\\cong_x\\mathbb R^3\\setminus B(0,\\frac12)\\) and such that \\(r|g_{ij}-\\delta_{ij}|+r^2|\\partial_kg_{ij}|+r^3|\\partial^2_kg_{ij}|\\leq C\\). For any initial data set \\((M,g)\\) there is a complete Riemannian manifold \\((\\widetilde M,\\widetilde g)\\) diffeomorphic to \\(\\mathbb R^3\\) that contains \\((M,g)\\) isometrically. A Borel set \\(U\\subset\\widetilde M\\) is said to contain the horizon if \\(\\widetilde M\\setminus M\\subset U\\). If \\(U\\) has locally finite perimeter, then its reduced boundary \\(\\partial^*U\\) of \\((\\widetilde M,\\widetilde g)\\) is supported in \\(M\\) and \\({\\mathcal H}^2_g(\\partial^*U)={\\mathcal H}^2_{\\widetilde g}(\\partial^*U)\\). The isoperimetric area function \\(A_g\\) is defined as \\(A_g(V)=\\inf\\{{\\mathcal H}^2_{g}(\\partial^*U)\\}\\), where \\(U\\subset\\widetilde M\\) is a Borel set containing the horizon and of finite perimeter with \\({\\mathcal L}_g^3(U)=V\\). A Borel set \\(\\Omega\\subset\\widetilde M\\) containing the horizon and of finite perimeter with \\({\\mathcal L}_g^3(U)=V\\) and \\(A_g(V)=\\inf\\{{\\mathcal H}^2_{g}(\\partial^*U)\\}\\) is called an isoperimetric region of \\((M,g)\\) of volume \\(V\\).  In this paper, the authors study the isoperimetric structure of asymptotically flat Riemannian 3-manifolds \\((M, g)\\) that are \\(\\mathcal{C}^0\\)-asymptotic to the Schwarzschild metric of mass \\(m>0\\). They show that if \\((M,g)\\) is an initial data set that is \\(C^0\\)-asymptotic to the Schwarzschild metric of mass \\(m>0\\), then there exists \\(V_0>0\\) such that for every \\(V\\geq V_0\\), the infimum in \\(A_g(V)\\) is achieved and every minimizer has a smooth bounded representative whose boundary consists of the horizon and a connected surface that is close to a centered coordinate sphere. Also, it is shown that if the initial data set \\((M,g)\\) is \\(C^4\\)-asymptotic to the Schwarzschild metric of mass \\(m>0\\), then the boundaries of the large isoperimetric regions coincide with the volume-preserving stable constant mean curvature surfaces. In particular, for every sufficiently large volume there exists a unique isoperimetric region in \\((M,g)\\) of that volume. The boundaries of these regions foliate the complement of a bounded subset of 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