Audio-visual interactions in green spaces are important for mental health and wellbeing. However, the influence of audio-visual interactions on psychological responses is still less clear. This study introduced a new method, namely the audio-visual walk (AV-walk), to obtain data on the audio-visual context, audio-visual experiences, and psychological responses in two typical parks, namely Cloves Park and Music Park in Harbin, China. Some interesting results are as follows: First, based on Pearson’s correlation analysis, sound pressure level and roughness were significantly correlated with psychological responses in Cloves Park (p < 0.05). Second, the results of stepwise regression models showed the impact intensity of acoustic comfort was 1.64–1.68 times higher than that of visual comfort on psychological responses of emotion dimension, while visual comfort was 1.35–1.37 times higher than acoustic comfort on psychological responses of cognition dimension in Music Park. In addition, an orthogonal analysis diagram explained the influence of audio-visual interactions on psychological responses of young people. The audio-visual context located beside the waterscape with a relatively higher level of acoustic and visual comfort was the most cheerful (2.60), relaxed (2.45), and energetic (2.05), while the audio-visual context close to an urban built environment tended to be both acoustically and visually uncomfortable, and the psychological state was decreased to the most depressed (−0.25), anxious (−0.75), fatigued (−1.13) and distracted (−1.13).