The study investigated the use of polyethylene terephthalate (rPET) fibers for strengthening construction materials. The addition of 0.5 vol% rPET fibers to mortar was studied, but the smooth surface of rPET resulted in weak bonds with the mortar matrix, leading to a decreased interfacial transfer zone (ITZ) compared to the surrounding matrix. To address this issue, nano-particle and NaOH hydrolysis were used to improve the ITZ bond strength and frictional behavior. Additionally, surface treatment of rPET using NaOH and silane coating was performed to enhance the hydrophilicity and bond strength with the matrix. The effects of seawater on the material were also studied using XRD. Additionally, cemGEMS analysis was also conducted. The SEM was used to observe the degree of bonding at the ITZ between rPET and the mortar matrix. The study showed that adding 0.5 vol% of rPET fibers had a significant impact on the tensile strength and fracture energy of mortar, and the fiber dispersibility was a crucial factor in controlling its mechanical properties. The low-cost recycled PET fibers were also found to be effective as a reinforcing agent in seawater-mixed mortar for marine applications, increasing the mortar's fracture energy by 188–802%. Therefore, these fibers can be used in coastal structures requiring impact-resistant non-metallic materials, such as wave-dissipating concrete blocks or marine concrete structures reinforced with non-corrosive materials like FRP.