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This paper studies the selection of valid and relevant moments for the generalized method of moments (GMM) estimation. For applications with many candidate moments, our asymptotic analysis accommodates a diverging number of moments as the sample size increases. The proposed procedure achieves three objectives in one-step: (i) the valid and relevant moments are distinguished from the invalid or irrelevant ones; (ii) all desired moments are selected in one step instead of in a stepwise manner; (iii) the parameters of interest are automatically estimated with all selected moments as opposed to a post-selection estimation. The new method performs moment selection and efficient estimation simultaneously via an information-based adaptive GMM shrinkage estimation, where an appropriate penalty is attached to the standard GMM criterion to link moment selection to shrinkage estimation. The penalty is designed to signal both moment validity and relevance for consistent moment selection. We develop asymptotic results for the high-dimensional GMM shrinkage estimator, allowing for non-smooth sample moments and weakly dependent observations. For practical implementation, this one-step procedure is computationally attractive. Download Paper