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To develop a fast, quantitative 3D magnetization transfer contrast (MTC) framework based on an unsupervised learning scheme, which will provide baseline reference signals for CEST and nuclear Overhauser enhancement imaging. Pseudo-randomized RF saturation parameters and relaxation delay times were applied in an MR fingerprinting framework to generate transient-state signal evolutions for different MTC parameters. Prospectively compressed sensing-accelerated (four-fold) MR fingerprinting images were acquired from 6 healthy volunteers at 3