•The LBL electrostatic deposition maintained strawberry firmness and volatile aroma.•The LBL coating inhibited some primary metabolism in strawberry.•Special secondary metabolites in LBL coated strawberry were reduced after storage. Postharvest strawberries (Fragaria × ananassa Duch.) were coated either by the layer-by-layer (LBL) electrostatic deposition, based on chitosan and carboxymethyl cellulose (CMC), or coated by 1% chitosan. Results suggested that LBL edible coating was significantly effective at inhibiting the loss of fruit firmness and aroma volatiles of strawberry, with little effect on the total soluble solids and total acidity contents. Through an untargeted metabolomic analysis, we found that the LBL application significantly reduced the primary metabolite contents involved in carbohydrate, fatty acids and amino acids metabolism, as well as the secondary metabolite contents involved in terpenoid, carotenoid, phenylpropanoid and flavonoid metabolism after storage. Our results indicated that the LBL edible coating could be potential to maintain strawberry quality with lower metabolites contents after eight days of storage.