Submodular extensions of an energy function can be used to efficiently compute approximate marginals via variational inference. The accuracy of the marginals depends crucially on the quality of the submodular extension. To identify the best possible extension, we show an equivalence between the submodular extensions of the energy and the objective functions of linear programming (LP) relaxations for the corresponding MAP estimation problem. This allows us to (i) establish the optimality of the submodular extension for Potts model used in the literature; (ii) identify the optimal submodular extension for the more general class of metric labeling; and (iii) efficiently compute the marginals for the widely used dense CRF model using a recently proposed Gaussian filtering method. Using both synthetic and real data, we show that our approach provides comparable upper bounds on the log-partition function to those obtained using tree-reweighted message passing (TRW) in cases where the latter is computationally feasible. Importantly, unlike TRW, our approach provides the first practical algorithm to compute an upper bound on the dense CRF model.