Carbon nanotube (CNT), as reinforcing agents in natural rubber (NR), has gained a large amount of consideration due to their excellent properties. Uniform dispersion of CNT is the key to obtaining high-performance NR nanocomposites. In this contribution, a novel ultrasonic grinding dispersion method of CNT with waterjet-produced rubber powder (WPRP) as a carrier is proposed. Microscopic morphologies show that a Xanthium-like structure with WPRP as the core and CNTs as the spikes is formed, which significantly improves the dispersion of CNT in the NR matrix and simultaneously strengthens the bonding of the WPRP and NR matrix. With the increase in the WPRP loading, the Payne effect of CNT/WPRP/NR composites decreases, indicating the effectiveness of the dispersion method. The vulcanization MH and ML value and crosslinking density increase with the increase in the WPRP loading, whereas the scorch time and cure time exhibit a decreasing trend when the WPRP loading is less than 15 phr. It is found that the CNT/WPRP/NR composites filled with 5 phr WPRP have a 4% increase in 300% modulus, a 3% increase in tensile strength, while a 5% decrease in Akron abrasion loss, compared to CNT/NR composites.