This study aimed to explore the influence of film thickness on the piezoelectric efficiency of polyvinylidene fluoride/graphitic carbon nitrate nanosheet (GCN) composite films, taking into account the effect of GCN alignment. Our findings demonstrated that the piezoelectric performance of these films was markedly dependent on their thickness. We have observed a direct relationship between film thickness and piezoelectric efficiency, with thicker films showing a greater capability to convert mechanical pressure into electric energy. This increased efficiency is attributed to the enhanced ability to thicker films to distribute stress uniformly across the material, which is crucial for optimizing the piezoelectric effect. Our results advance the understanding of how variation in film thickness impact mechanical properties such as stiffness and flexibility, which subsequently affect the piezoelectric response. Through predictive modeling, we analyzed the mechanical dynamics of film displacement under an electrical potential and clarified how different thickness influenced the mechanical properties and piezoelectric output. This detailed analysis deepens the fundamental understanding of material design for optimal piezoelectric performance and underscores the critical role of film thickness in engineering application.