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The iterative method is an important way to solve the generalized coupled Sylvester systems. In this paper, an iterative algorithm is constructed to solve the minimum Frobenius norm residual problem: \\(||(\\binom{AXB}{CXD}) - (\\binom EF)|| = \\min\\) over a generalized reflexive matrix \\(X\\). For any initial generalized reflexive matrix \\(X_1\\), by the iterative algorithm, the generalized reflexive solution \\(X^\\ast\\) can be obtained within finite iterative steps in the absence of round-off errors, and the unique least-norm generalized reflexive solution \\(X^\\ast\\) can also be derived when an appropriate initial iterative matrix is chosen. Furthermore, the unique optimal approximate solution \\(\\hat X\\) to a given matrix \\(X_0\\) in Frobenius norm can be derived by finding the least-norm generalized reflexive solution \\(\\widetilde X^\\ast\\) of a new corresponding minimum Frobenius norm residual problem: \\(\\min || (\\binom{A\\widetilde{X}B}{C\\widetilde{X}D}) - (\\binom{\\widetilde{E}}{\\widetilde{F}})\\) with \\(\\widetilde{E} = E - AX_0B, \\widetilde{F} = F - CX_0D\\). Finally, several numerical examples are given to illustrate that our iterative algorithm is 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