To study the alteration pattern and defensive response mechanism triggered by herbivorous feeding stimuli under natural conditions, we built a biological model of the interrelationship between the Chinese pine (Pinus tabuliformis Carr.) and the Chinese pine caterpillar (Dendrolimus tabulaeformis Tsai et Liu) within their native habitat. We integrated proteomic and phosphoproteomic data, normalized the results, and combined them with bioinformatics to evaluate and analyze variations in phosphoproteomics in pine needles' response to the caterpillar's feeding stimulus. We systematically identified differentially significant phosphorylated proteins implicated in the pine's defense mechanism against caterpillar stress. Furthermore, we predicted upstream kinases of phosphorylation sites and their activities. Similarly, through an analysis of the Motif patterns of phosphorylated proteins, Mfuzz clustering of phosphorylation sites, kinase regulatory networks and functional modules of phosphorylated protein interaction networks in response to stress within pine, we can investigate the mechanisms behind resistance formation and regulation of caterpillar feeding incentives in pine. The identification results of partially phosphorylated proteins were additionally confirmed through PRM technology. Furthermore, genes upstream of differentially expressed proteins were validated through RT-qPCR detection.