We propose a method for solving three-dimensional boundary value problems for Laplace’s equation in an unbounded domain. It is based on non-overlapping decomposition of the exterior domain into two subdomains so that the initial problem is reduced to two subproblems, namely, exterior and interior boundary value problems on a sphere. To solve the exterior boundary value problem, we propose a singularity isolation method. To match the solutions on the interface between the subdomains (the sphere), we introduce a special operator equation approximated by a system of linear algebraic equations. This system is solved by iterative methods in Krylov subspaces. The performance of the method is illustrated by solving model problems.