Effective antioxidants and reinforcing fillers are essential to addressing the aging and toughness issues of elastomers. Inspired by the toughness of mussels and excellent anti-aging properties of materials containing –OH and/or –NH2groups, we synthesized eco-friendly polydopamine-loaded silica (silica-PDA) particles via a one-pot-synthesis approach using ceric ammonium nitrate (CAN) as the catalyst. The silica-PDA particles, which were well dispersed in the natural rubber matrix, simultaneously improved the toughness and slowed the aging process of the matrix. Compared to neat NR, the Silica-PDA composite had enhanced mechanical performance and interfacial interaction at the low loading percentage of the silica-PDA particles. The tensile strength of the Silica-PDA composite was 40.4% higher than that of neat NR, and the fracture energy of the composite was 354 kJ m−2.