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Magnetic resonance (MR) fingerprinting is a new quantitative imaging paradigm, which simultaneously acquires multiple MR tissue parameter maps in a single experiment. In this paper, we present an estimation-theoretic framework to perform experiment design for MR fingerprinting. Specifically, we describe a discrete-time dynamic system to model spin dynamics, and derive an estimation-theoretic bound, i.e., the Cramér-Rao bound, to characterize the signal-to-noise ratio (SNR) efficiency of an MR fingerprinting experiment. We then formulate an optimal experiment design problem, which determines a sequence of acquisition parameters to encode MR tissue parameters with the maximal SNR efficiency, while respecting the physical constraints and other constraints from the image decoding/reconstruction process. We evaluate the performance of the proposed approach with numerical simulations, phantom …