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Homotopy Relat. Struct. 4, No.~1, 187--244 (2009; Zbl 1189.53026)], the authors established an isomorphism between the categories \\(\\text{Funct}^{\\infty}({\\mathcal P}_1(X), {\\mathcal B}G)\\) and \\(Z^1_X(G)^{\\infty}\\). In this respect, given a smooth manifold \\(X\\) and a Lie group \\(G\\), \\(\\text{Funct}^{\\infty}({\\mathcal P}_1(X), {\\mathcal B}G)\\) is the category of smooth functors from the path-groupoid \\({\\mathcal P}_1(X)\\) to the Lie groupoid \\({\\mathcal B}G\\) (i.e., the category with one object whose set of morphisms is the Lie group \\(G\\)), while \\(Z^1_X(G)^{\\infty}\\) is the category whose objects are the 1-forms \\(A \\in \\Omega^1(X,{\\mathfrak g})\\) on \\(X\\) with values in the Lie algebra \\({\\mathfrak g}\\) of \\(G\\) and whose morphisms \\(g : A \\to A'\\) are the smooth functions \\(g : X \\to G\\) satisfying  \\[  A' = \\text{Ad}_g(A) - g^*(\\bar{\\theta}),  \\]  where \\(\\bar{\\theta}\\) is the right-invariant Maurer-Cartan form on \\(G\\).  In the present paper, the above isomorphism is generalized to 2-functors and 2-forms. Thus, the 2-categories \\({\\mathcal P}_2(X)\\) and \\({\\mathcal B}{\\mathfrak G}\\) are introduced to replace \\({\\mathcal P}_1(X)\\) and \\({\\mathcal B}G\\). The path 2-groupoid \\({\\mathcal P}_2(X)\\) is obtained by adding 2-morphisms to \\({\\mathcal P}_1(X)\\), and \\({\\mathcal B}{\\mathfrak G}\\) is the 2-category with one object whose set of morphisms is the 2-group \\({\\mathfrak G}\\) (i.e., two groups \\(G\\), \\(H\\), with additional structure). The main result of the paper is the equivalence of the smooth 2-functors in \\(\\text{Funct}^{\\infty}({\\mathcal P}_2(X), {\\mathcal B}{\\mathfrak G})\\) with the pairs \\((A,B) \\in \\Omega^1(X,{\\mathfrak g}) \\times \\Omega^2(X,{\\mathfrak h})\\), where \\({\\mathfrak g}\\) and \\({\\mathfrak h}\\) are the Lie algebras of \\(G\\) and \\(H\\) and \\(A\\), \\(B\\) satisfy  \\[  dA + [A \\wedge A] = t_*(B).  \\]   Three examples of smooth 2-functors are given in Section 4. They appear as connections on non-abelian gerbes, as derivatives of smooth functors and as critical points in BF theory. A generalization of the main result to diffeological spaces is given in Section 5.  The paper contains appendices on 2-categories, and on 2-groups and crossed 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