Subunit models provide a powerful yet parsimonious description of neural spike responses to complex stimuli. They can be expressed by a cascade of two linear-nonlinear (LN) stages, with the first linear stage defined by convolution with one or more filters. Recent interest in such models has surged due to their biological plausibility and accuracy for characterizing early sensory responses. However, fitting subunit models poses a difficult computational challenge due to the expense of evaluating the log-likelihood and the ubiquity of local optima. Here we address this problem by forging a theoretical connection between spike-triggered covariance analysis and nonlinear subunit models. Specifically, we show that a ''convolutional'' decomposition of the spike-triggered average (STA) and covariance (STC) provides an asymptotically efficient estimator for the subunit model under certain technical conditions. We also prove the identifiability of such convolutional decomposition under mild assumptions. Our moment-based methods outperform highly regularized versions of the GQM on neural data from macaque primary visual cortex, and achieves nearly the same prediction performance as the full maximum-likelihood estimator, yet with substantially lower cost.