High-strength-high-modulus polyimide (PI) cords reinforced natural rubber (NR) composites are prepared, and the PI cords are treated with resorcinolformaldehyde-latex (RFL) adhesive to enhance the interfacial adhesion with NR matrix. The influence of RFL adhesive variables, such as the ratio of R/F and RF/L, on the adhesion between PI cords and NR is investigated. Furthermore, sorbitol glycidyl ether (SGE) and caprolactam blocked methylene diisocyanate (CBI) are adhered to the surface of the PI cords through a dipcoating procedure to introduce epoxy and NCO groups and graft with more RFL adhesive. The H pull-out force of SGE/CBI-RFL treated PI cords/NR composites reaches as high as 193.9 N, which is 580% higher than that of untreated PI ones. Additionally, the SGE/CBI-RFL treated PI cords/NR composites exhibit superior adhesion, aging, and fatigue resistance together with better mechanical properties as compared with SGE/CBI-RFL treated poly(paraphenylene terephtalamide) (PPTA) cords/NR composites.