Muscular control during walking is believed to be simplified by the coactivation of muscles called muscle synergies. Although significant corticomuscular connectivity during walking has been reported, the level at which the cortical activity is involved in muscle activity (muscle synergy or individual muscle level) remains unclear. Here we examined cortical correlates of muscle activation during walking by brain decoding of activation of muscle synergies and individual muscles from electroencephalographic signals. We demonstrated that the activation of locomotor muscle synergies was decoded from slow cortical waves. In addition, the decoding accuracy for muscle synergies was greater than that for individual muscles and the decoding of individual muscle activation was based on muscle-synergy-related cortical information. These results indicate the cortical correlates of locomotor muscle synergy activation. These findings expand our understanding of the relationships between brain and locomotor muscle synergies and could accelerate the development of effective brain-machine interfaces for walking rehabilitation.