The purpose of this study was to develop an integrated control strategy for multiscale crystallization processes. An image analysis method using a deep learning neural network is used to measure the fine-scale information of the crystallization process, and the mathematical statistical method is adopted to obtain the mean size of the crystal population. A feedforward neural network is subsequently trained and employed in a nonlinear model predictive control formulation to obtain the optimal profile of the manipulated variable. The effectiveness of the proposed nonlinear model predictive control method is evaluated using alum cooling crystallization experiments. Experimental results demonstrate benefits of the proposed combination of feedforward neural network and nonlinear model predictive control method for the multiscale crystallization process.