Human beings have a long history of understanding, exploring, and pursuing music and health, and ancient and modern cultures have provided detailed and clear records of this. We here attempt to examine the effects of music on individuals’ emotional experiences and psychophysiological signals by exploring the functions of music at both the psychological and physiological levels. The present study investigated the mood induced by popular music from a psychological and physiological measurement perspective, focusing on the effects of the following factors on mood: key (major, minor, pentatonic); rhythmic pattern (steady rhythm, flowing rhythm), and a total of 40 subjects were recruited for the study. Psychophysiological signals under the influence of music were measured and analyzed. The results showed that: tonality had a significant effect on arousal and potency, and pentatonic tonality had a significant difference in a poetic sense and heart rate variability from Western tonality; the rhythmic type had a significant effect on arousal and poetic sense; in the presence of musical stimuli only, theta power spectral moments were significantly different in the left and right hemispheres, and the right side was larger than the left side; theta power spectra differed with different tonality and rhythmic type: theta power The theta power spectrum differs with different tunings and rhythmic patterns: the difference between left and right brain is smaller in pentatonic than in Western tuning. Therefore, music has significant effects on both emotion and physiological psychology, and the theoretical and methodological findings of this study lay the foundation for the design of musical interaction services.