An important challenge in the study of functional corticomuscular coupling (FCMC) is an accurate capture of the coupling relationship between the cerebral cortex and the effector muscle. The coherence method is a linear analysis method, which has certain limitations in further revealing the nonlinear coupling between neural signals. Although mutual information (MI) and transfer entropy (TE) based on information theory can capture both linear and nonlinear correlations, the equitability of these algorithms is ignored and the nonlinear components of the correlation cannot be separated. The maximal information coefficient (MIC) is a suitable method to measure the coupling between neurophysiological signals. This study extends the MIC to the time–frequency domain, named time–frequency maximal information coefficient (TFMIC), to explore the FCMC in a specific frequency band. The effectiveness, equitability, and robustness of the algorithm on the simulation data was verified and compared with coherence, TE- and MI- based methods. Simulation results showed that the TFMIC could accurately detect the coupling for different functional relationships at low noise levels. The dorsiflexion experimental results revealed that the beta-band (14–30 Hz) significant coupling was observed at channels Cz, C4, FC4, and FCz. Additionally, the results showed that the coupling was higher in the alpha-band (8–13 Hz) and beta-band (14–30 Hz) than in the gamma-band (31–45 Hz). This might be related to a transition between sensorimotor states. Specifically, the nonlinear component of FCMC was also observed at channels Cz, C4, FC4, and FCz. This study expanded the research on nonlinear coupling components in FCMC.