In the aluminum reduction process, aluminum fluoride (AlF3) is added to lower the liquidus temperature of the electrolyte and increase the electrolytic efficiency. Making the decision on the amount of AlF3 addition (referred to in this work as MDAAA) is a complex and knowledge-based task that must take into consideration a variety of interrelated functions; in practice, this decision-making step is performed manually. Due to technician subjectivity and the complexity of the aluminum reduction cell, it is difficult to guarantee the accuracy of MDAAA based on knowledge-driven or data-driven methods alone. Existing strategies for MDAAA have difficulty covering these complex causalities. In this work, a data and knowledge collaboration strategy for MDAAA based on augmented fuzzy cognitive maps (FCMs) is proposed. In the proposed strategy, the fuzzy rules are extracted by extended fuzzy k-means (EFKM) and fuzzy decision trees, which are used to amend the initial structure provided by experts. The state transition algorithm (STA) is introduced to detect weight matrices that lead the FCMs to desired steady states. This study then experimentally compares the proposed strategy with some existing research. The results of the comparison show that the speed of FCMs convergence into a stable region based on the STA using the proposed strategy is faster than when using the differential Hebbian learning (DHL), particle swarm optimization (PSO), or genetic algorithm (GA) strategies. In addition, the accuracy of MDAAA based on the proposed method is better than those based on other methods. Accordingly, this paper provides a feasible and effective strategy for MDAAA.