We consider the problem of learning function classes computed by neural networks with various activations (e.g. ReLU or Sigmoid), a task believed to be computationally intractable in the worst-case. A major open problem is to understand the minimal assumptions under which these classes admit provably efficient algorithms. In this work we show that a natural distributional assumption corresponding to eigenvalue decay of the Gram matrix yields polynomial-time algorithms in the non-realizable setting for expressive classes of networks (e.g. feed-forward networks of ReLUs). We make no assumptions on the structure of the network or the labels. Given sufficiently-strong polynomial eigenvalue decay, we obtain fully-polynomial time algorithms in all the relevant parameters with respect to square-loss. Milder decay assumptions also lead to improved algorithms. This is the first purely distributional assumption that leads to polynomial-time algorithms for networks of ReLUs, even with one hidden layer. Further, unlike prior distributional assumptions (e.g., the marginal distribution is Gaussian), eigenvalue decay has been observed in practice on common data sets.