Travel mode choice (TMC) prediction is crucial for transportation planning. Most previous studies have focused on TMC in adults, whereas predicting TMC in children has received less attention. On the other hand, previous children’s TMC prediction studies have generally focused on home-to-school TMC. Hence, LIGHT GRADIENT BOOSTING MACHINE (LGBM), as a robust machine learning method, is applied to predict children’s TMC and detect its determinants since it can present the relative influence of variables on children’s TMC. Nonetheless, the use of machine learning introduces its own challenges. First, these methods and their performance are highly dependent on the choice of “hyperparameters”. To solve this issue, a novel technique, called multi-objective hyperparameter tuning (MOHPT), is proposed to select hyperparameters using a multi-objective metaheuristic optimization framework. The performance of the proposed technique is compared with conventional hyperparameters tuning methods, including random search, grid search, and “Hyperopt”. Second, machine learning methods are black-box tools and hard to interpret. To overcome this deficiency, the most influential parameters on children’s TMC are determined by LGBM, and logistic regression is employed to investigate how these parameters influence children’s TMC. The results suggest that MOHPT outperforms conventional methods in tuning hyperparameters on the basis of prediction accuracy and computational cost. Trip distance, “walkability” and “bikeability” of the origin location, age, and household income are principal determinants of child mode choice. Furthermore, older children, those who live in walkable and bikeable areas, those belonging low-income groups, and short-distance travelers are more likely to travel by sustainable transportation modes.