The mechanism is studied to optimize the cultivation of piano talents and entrepreneurial psychological quality (PSYQ) in colleges and universities through the QS (Questionnaire Survey). Firstly, the cultivation of piano talents’ entrepreneurial consciousness is explored, together with the entrepreneurial will, entrepreneurial personality, and entrepreneurial ability. Secondly, the piano talents entrepreneurial PSYQ training model is established according to the internal factors of college students majoring in piano, entrepreneurial attitude, students’ interpersonal network, and entrepreneurial environment factors. The correlations between various variables are analyzed. Afterward, a QS is designed, and the data are collected from university A in the city of Xi’an. Data analysis shows significant differences in the cultivation of entrepreneurial PSYQ among students of different grades in college Piano Majors, namely, p < 0.01. Students growing up in different environments show significant differences in entrepreneurial PSYQ, namely, p < 0.01. Meanwhile, whether students have served as cadres will also have a particular impact on students’ entrepreneurial PSYQ, namely, p < 0.01. However, the dimension of only-child-or-not in entrepreneurial PSYQ training does not show a significant difference. Finally, under the model analysis, achievement motivation, entrepreneurial attitude, entrepreneurial interest, entrepreneurial consciousness, interpersonal network, entrepreneurial environment, and personal entrepreneurial background will affect the cultivation of their entrepreneurial PSYQ. They show a positive correlation with the entrepreneurial PSYQ. Therefore, in the future college piano talents training and entrepreneurial PSYQ training, more focus should be put on students’ innovative thinking and risk challenging capacity, thereby helping students with better entrepreneurial work.