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A Casselman-Wallach representation of \\(G\\) is a smooth Harish-Chandra representation of moderate growth on a Fr\u00e9chet space. Let \\(U^\\infty\\) and \\(V^\\infty\\) be a pair of Casselman-Wallach representations of \\(G\\) which are contragredient to each other, and let \\(\\langle\\;,\\;\\rangle:U^\\infty\\times V^\\infty\\to\\mathbb C\\) be the corresponding \\(G\\)-invariant bilinear map. For \\(u\\in U^\\infty\\) and \\(v\\in V^\\infty\\), the matrix coefficient \\(c_{u\\otimes v},g\\mapsto\\langle gu,v\\rangle\\) is a tempered function on \\(G\\). Let \\(U^{-\\infty}\\) and \\(V^{-\\infty}\\) denote the strong duals of \\(V^{\\infty}\\) and \\(U^\\infty\\), respectively. These spaces carry smooth Harish-Chandra representations whose underlying Harish-Chandra modules are infinitesimally equivalent to those of \\(U^\\infty\\) and \\(V^\\infty\\), resp. Let \\(C^\\xi(G)\\) and \\(C^{-\\xi}(G)\\) be the space of tempered functions, and the space of tempered generalized functions on \\(G\\) (i.e., the space of continuous linear functionals on the space of Schwartz densities on \\(G\\)), respectively. Then \\(U^\\infty\\), \\(V^\\infty\\), and \\(C^\\xi(G)\\) embed into \\(U^{-\\infty}\\), \\(V^{-\\infty}\\), and \\(C^{-\\xi}(G)\\), respectively.   The first main result of this paper formalizes the notion of matrix coefficients for distributional vectors. It asserts that the matrix coefficient map \\(c: U^\\infty\\times V^\\infty\\to C^\\xi(G)\\) extends to a continuous bilinear map \\(U^{-\\infty}\\times V^{-\\infty}\\to C^{-\\xi}(G)\\), and that the induced \\(G \\times G\\) intertwining map \\(U^{-\\infty}\\otimes V^{-\\infty}\\to C^{-\\xi}(G)\\) is a topological homomorphism with closed image.  As an application, the authors then prove a generalized form of the Gelfand-Kazhdan criterion for real reductive 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