Finding the optimal parameters in laser processing applications can be time-consuming given the large parameter space and various sources of error. This problem is exacerbated by day-to-day variation in laser beam characteristics and a large variety of materials that need to be processed. The ideal laser processing system should be “smart,” meaning that it can sense changes in the environment, make proper adjustment, and predict parameters for new materials. As a step toward this goal, we propose a method to efficiently extract the areas of a large number of laser-induced damages in situ using an automated data acquisition system that can control laser parameters, motorized stage movement, image capturing/processing, and feature extraction. The damage areas are extracted and compared with direct measurements. Damage areas are fed into an artificial neural network (ANN) for prediction. Various ANN structures and training functions are tested to create the optimal ANN for prediction. ANN predictions were found to be capable enough to accurately model and optimize the laser processing parameters that were investigated. With the capability of collecting a large amount of usable data in a short period of time, this acquisition system can be used to train sophisticated ANNs for complicated tasks such as quality control and failure prediction.