Controlled islanding is an effective remedy to prevent large-area blackouts in a power system under a critically unstable condition. When and where to separate the power system are the essential issues facing controlled islanding. In this paper, both tasks are studied to ensure higher time efficiency and a better post-splitting restoration effect. A transient stability assessment model based on extreme learning machine (ELM) and trajectory fitting (TF) is constructed to determine the start-up criterion for controlled islanding. This model works through prompt stability status judgment with ELM and selective result amendment with TF to ensure that the assessment is both efficient and accurate. Moreover, a splitting surface searching algorithm, subject to minimal power disruption, is proposed for determination of the controlled islanding implementing locations. A highlight of this algorithm is a proposed modified electrical distance concept defined by active power magnitude and reactance on transmission lines that realize a computational burden reduction without feasible solution loss. Finally, the simulation results and comparison analysis based on the New England 39-bus test system validates the implementation effects of the proposed controlled islanding strategy.