We report on our recent attempt to pioneer “multicrystalline informatics” through collaboration of experiments, theory, computation, and machine learning to establish universal guidelines how we can obtain high-performance multicrystalline materials. We employ silicon as a model material, and develop various useful machine learning models. One example is a neural network to predict distribution of crystal orientations in a large-area sample from multiple optical images. Transfer learning of pre-trained image classifier could predict spatial distribution of probability of dislocations generation from photoluminescence images. Extracted regions with high probability of dislocations generation could be characterized by multiscale experiments as well as computation using artificial-neural-network interatomic potential to disclose the physics behind. The obtained knowledge could be useful for process development of high-performance multicrystalline materials.