The phyllosphere encompasses all above-ground plant surfaces, covering ~10 9 km 2 globally and hosting up to 10 26 microbial cells, yet its chemical ecology remains understudied compared to the rhizosphere. This review synthesizes recent advances in metabolite-mediated communication orchestrating phyllosphere microbiome assembly, function, and host feedback. Leaf structural traits, host immune genes, developmental stage, and fluctuating environmental drivers create spatiotemporal chemical niches that filter incoming microbes. We then examine four major classes of plant derived signals, including primary metabolites, secondary metabolites, phytohormones and volatile organic compounds, and we emphasize their dual roles. Microbial feedback occurs through phytohormone synthesis/catabolism, volatile and soluble effectors, and antimicrobial metabolites that collectively modulate plant immunity, growth, and stress tolerance while structuring inter-microbial competition. These bidirectional exchanges form a dynamic network where plants and microbes continuously negotiate cooperation and conflict under diurnal and seasonal oscillations. We outline translational prospects including probiotic foliar applications, metabolite priming, and breeding for beneficial consortia, while identifying key challenges in signal attribution, microbiota stabilization, and deciphering community-level crosstalk dynamics for sustainable crop protection.