Emerging evidence has confirmed the role of emerging nonthermal stressors (e.g., electromagnetic fields, ultrasonication, plasma) in accumulating bioactive metabolites in plant-based food. However, the signal decoding mechanisms behind NonTt-driven phytochemical production remain unclear, hindering postharvest bioactive component intensification. This study aims to summarize the association between signaling molecules and bioactive secondary metabolite production under nonthermal conditions, demonstrating the feasibility of enhancing phytochemical accumulation through signaling molecule crosstalk manipulation. Nonthermal elicitors were found to be capable of inducing stress metabolisms and activating various signaling molecules, similar to conventional abiotic stress. A simplified pathway model for nonthermally induced γ-aminobutyric acid accumulation was proposed with reactive oxygen species and calcium signaling being versatile pathways responsive to nonthermal elicitors. Manipulating signal molecules/pathways under nonthermal conditions can intensify phytochemical biosynthesis. Further research is needed to integrate signaling molecule responses and metabolic network shifts in nonthermally stressed plant-based matrices, balancing quality modifications and intensification of food functionality potential.