Designing polymeric membranes with high solute−solute selectivity and permeance is important but technically challenging. Existing industrial interfacial polymerization (IP) process to fabricate polyamide-based polymeric membranes is largely empirical, which requires enormous trial-and-error experimentations to identify optimal fabrication conditions from a wide candidate space for separating a given solute pair. Herein, we developed a novel multitask machine learning (ML) model based on an artificial neural network (ANN) with skip connections and selectivity regularization to guide the design of polyamide membranes. We used limited sets of lab-collected data to obtain satisfactory model performance over four iterations by introducing human expert experience in the online learning process. Four membranes under fabrication conditions guided by the model exceeded the present upper bound for mono/divalent ion selectivity and permeance of the polymeric membranes. Moreover, we obtained new mechanistic insights into the membrane design through feature analysis of the model. Our work demonstrates a ML approach that represents a paradigm shift for high-performance polymeric membranes design.