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It is possible to prevent collapse of the whole post-fault power system, which is in unstable condition, by determining the splitting boundary so as to calm down the system oscillation. A fast method of searching for the splitting boundary of power system controlled islanding is presented in this paper, the aim of which is to minimize the load-generation imbalance in each island. The method contains three phases, namely, defining the domain of each generator according to power flow tracing algorithm, determining an initial splitting boundary based on the grouping information of generators, and refining the initial one to get the final splitting boundary. A real-time searching program for power system splitting boundary was developed based on the method. Simulations on the IEEE 118-bus power system and a practical power system show that the proposed method is effective and fast.