The poroelastic road surface (PERS) mixture with low polyurethane content (PERS-LPC) can reduce the construction cost of PERS pavement, which exhibits promising noise reduction capacity, whereas its mechanical performance needs to be further enhanced for real practice. This study aims to investigate the effectiveness of surface activations of crumb rubber and aggregate to improve the mechanical performance of PERS-LPC. Molecular dynamics (MD) simulations and indoor experiments have been conducted, including the indirect tension (IDT) test implemented on the dry-cured and freeze–thaw PERS-LPC specimens and Cantabro test performed on water-bathed specimens. The results showed that, the oxygen-containing groups, introduced by UV irradiation and KMnO4 soaking, enhanced surface polarity of crumb rubber and rubber-polyurethane bonding strength. The surface activity of basalt aggregate was increased by the inclusion of Portland cement but not by hydrated lime. The IDT strength of the dry-cured PERS-LPC mixture was improved by 10.3–17.5% with activated rubbers and by 35.6% with activated aggregates. The tension strength ratio (TSR) of the freeze–thaw mixture was increased only by 2% with activated rubber but up to 20.8% by the inclusion of 0.5 wt% cement. The Cantabro abrasion loss (CAL) of PERS-LPC specimens was reduced significantly from 20.1% to 11.6% with the soaked rubber and dropped dramatically to 7.9% after inclusion of 0.5 wt% cement. It was recommended to activate crumb rubber with UV irradiation for 24 h and mineral aggregate with 0.5 wt% cement in PERS-LPC mixture in terms of performance enhancement and operation convenience. The findings of this research were expected to support the mix design of an inexpensive and durable PERS-LPC mixture for noise reduction.