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Accumulating evidence from human-based research has highlighted that the prevalent one-size-fits-all approach for neural and behavioral interventions is inefficient. This approach can benefit one individual, but be ineffective or even detrimental for another. Studying the efficacy of the large range of different parameters for different individuals is costly, time-consuming and requires a large sample size that makes such research impractical and hinders effective interventions. Here an active machine learning technique is presented across participants—personalized Bayesian optimization (pBO)—that searches available parameter combinations to optimize an intervention as a function of an individual’s ability. This novel technique was utilized to identify transcranial alternating current stimulation (tACS) frequency and current strength combinations most likely to improve arithmetic performance, based on a subject’s baseline arithmetic abilities. The pBO was performed across all subjects tested, building a model of subject performance, capable of recommending parameters for future subjects based on their baseline arithmetic ability. pBO successfully searches, learns, and recommends parameters for an effective neurointervention as supported by behavioral, simulation, and neural data. The application of pBO in human-based research opens up new avenues for personalized and more effective interventions, as well as discoveries of protocols for treatment and translation to other clinical and non-clinical domains., Author summary The common one-size-fits-all approach used in biological and behavioral research has shown to be inefficient. This is especially the case in the field of brain stimulation, where many different combinations of stimulation parameters (i.e., frequency and current strength of the applied current) can be used for restorative or enhancement purposes, in clinical and non-clinical populations, respectively. Even intervention protocols that have reported to be effective for certain individuals can be detrimental for others. Here we present an active machine learning method, personalized Bayesian optimization (pBO) that successfully searches, learns, and recommends neurostimulation parameters across individuals. Based on an individual’s baseline cognitive ability, the pBO identifies specific combinations of transcranial alternating current stimulation parameters, which are most likely to improve cognitive performance, in which case arithmetic problem solving. This timely approach provides a possible solution for the pressing need for personalization in different disciplines including medicine, psychology, and education.