Wearable robotic devices have been shown to substantially reduce the energy expenditure of human walking. However, response variance between participants for fixed control strategies can be high, leading to the hypothesis that individualized controllers could further improve walking economy. Recent studies on human-in-the-loop (HIL) control optimization have elucidated several practical challenges, such as long experimental protocols and low signal-to-noise ratios. Here, we used Bayesian optimization—an algorithm well suited to optimizing noisy performance signals with very limited data—to identify the peak and offset timing of hip extension assistance that minimizes the energy expenditure of walking with a textile-based wearable device. Optimal peak and offset timing were found over an average of 21.4 ± 1.0 min and reduced metabolic cost by 17.4 ± 3.2% compared with walking without the device (mean ± SEM), which represents an improvement of more than 60% on metabolic reduction compared with state-of-the-art devices that only assist hip extension. In addition, our results provide evidence for participant-specific metabolic distributions with respect to peak and offset timing and metabolic landscapes, lending support to the hypothesis that individualized control strategies can offer substantial benefits over fixed control strategies. These results also suggest that this method could have practical impact on improving the performance of wearable robotic devices.