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The increasing need for engineered alloy nanoparticles (NPs) in diverse fields has spurred efforts to explore efficient/green synthesis methods. In this respect, spark ablation provides a scalable and viable way for producing widely different types of mixed NPs. Most importantly, implementation of the spark has the great advantage to combine a wider range of materials, thereby allowing the synthesis of mixed NPs with virtually unlimited combinations. Here we show that polarity reversal of spark discharges between two electrodes consisting of different materials enables synthesis of alloy NPs, while having a good potential to control the broadness of their composition distribution. A model developed in this work provides a tool for tuning the ablation ratio between the electrodes by adjusting the electric characteristics of the spark circuit. The ablation ratio is equal to the mean composition of the resulting NPs. The model predictions are in accordance with measurements obtained here and in earlier works. The unique way of producing alloy NPs by spark ablation shown in this work becomes especially useful when the starting electrode materials are immiscible at macroscopic scale. Copyright © 2018 American Association for Aerosol Research