Essential oil (EO) extraction is a widespread practice generating huge amounts of solid plant by-products a potential source of bioactive compounds, on the one hand, and a detrimental risk for the environment that needs to be carefully considered on the other hand. The present study aims to valorize Myrtus communis L. leaf by-products obtained following EO extraction using a steam distillation unit through the recovery of phenolic compounds and the evaluation of their biological activities. The total phenols, flavonoids, and proanthocyanidins contents of the ethanolic extract by-product were higher than the control (leaves without extraction of EO). Their amounts increased from 69.30 to 88.06 mg GAE/g for total phenols, from 36.31 to 70.97 mg QE for flavonoids and from 19.74 to 21.49 mg CE/g of extract for proanthocyanidins. The identification of phenolic compounds by high-performance liquid-chromatography equipped with a reversed-phase (RP-HPLC) system revealed that the by-product sample includes more gallic acid, catechin, syringic acid and luteolin 7-O-glucoside but less p-coumaric acid and kaempferol than the control. Moreover, the mid-infrared spectroscopy (MIR) showed the presence of benzene ring characteristic of phenolic compounds at 756 cm⁻¹, esters of aromatic acids and stretching vibrations of polyphenols at 1141–1234 cm⁻¹, C=C stretching present in phenolic acids such as coumaric acid and catechin at 1604 cm⁻¹. The assessment of antioxidant activity revealed that the ABTS^+• radical scavenging activity was significantly increased, whereas the DPPH^• radical inhibition activity and the ferric reduction antioxidant power were significantly decreased. The results indicated, as well, that Myrtus communis L. leaf by-products maintained a considerable antibacterial activity depending on the tested bacterial strain. Additionally, the anti-α-amylase activity was higher for the Myrtus communis L. leaf by-product extract. Therefore, Myrtus communis L. leaf by-products of EO extraction offer phenolic compounds with significant biological activities, contributing to the sustainable development and the promotion of circular economy by the recovery of valuable inputs from plant by-products.