We present a general framework for constructing prior distributions with structured variables. The prior is defined as the information projection of a base distribution onto distributions supported on the constraint set of interest. In cases where this projection is intractable, we propose a family of parameterized approximations indexed by subsets of the domain. We further analyze the special case of sparse structure. While the optimal prior is intractable in general, we show that approximate inference using convex subsets is tractable, and is equivalent to maximizing a submodular function subject to cardinality constraints. As a result, inference using greedy forward selection provably achieves within a factor of (1-1/e) of the optimal objective value. Our work is motivated by the predictive modeling of high-dimensional functional neuroimaging data. For this task, we employ the Gaussian base distribution induced by local partial correlations and consider the design of priors to capture the domain knowledge of sparse support. Experimental results on simulated data and high dimensional neuroimaging data show the effectiveness of our approach in terms of support recovery and predictive accuracy.