Ankle moment plays an important role in human gait analysis, patients' rehabilitation process monitoring, and the human-machine interaction control of exoskeleton robots. However, current ankle moment estimation methods mainly rely on inverse dynamics (ID) based on optical motion capture system (OMC) and force plate. These methods rely on fixed instruments in the laboratory, which are difficult to be applied to the control of exoskeleton robots. To solve this problem, this paper developed a new distributed plantar pressure system and proposed an ankle plantar flexion moment estimation method using the plantar pressure system. We integrated eight pressure sensors in each insole to collect the pressure data of the key area of the foot and then used the plantar pressure data to train four neural networks to obtain the ankle moment. The performance of the models was evaluated using normalized root mean square error (NRMSE) and cross-correlation coefficient (ρ). During experiments, eight subjects were recruited for the overground walking tests, and OMC and force plate were used as the gold standard. The results indicate that the Genetic algorithm - Gated recurrent unit estimation algorithm (GA-GRU) was the best estimation model which achieved the highest accuracy in generalized ankle moment estimation (NRMSE = 7.23%, ρ = 0.85) compared with the other models. The designed novel distributed plantar pressure system and the proposed method could serve as a joint moment estimation approach in wearable robot control and human motion state monitoring.