Ultrafine carboxylated Styrene-butadiene rubber(CSBR) powders were prepared by using gamma irradiation and following spray-drying method. The influences of dose rate, absorbed dose, and sensitizer content on the crosslinking density of CSBR latices were studied in detail. Then the ultrafine CSBR powders were used to toughen nylon 6. The toughness and thermal properties of nylon 6/CSBR blends were measured by using notched Izod impact test and differential scanning calorimetry and thermogravimetry, respectively. Results showed that the crosslinking density of CSBR increased with increasing of dose and sensitizer content, and it is independent on dose rate. The notched Izod impact strength of nylon 6 under room temperature increased after incorporation of irradiation crosslinked CSBR powders with appropriate crosslinking density. The morphology of higher impact nylon 6/CSBR blends indicated that the finer dispersion existed with dispersed particles of 150-nm diameter. Fracture morphology of nylon 6/CSBR blend suggested that the shear yielding in matrix is the primary toughening mechanism for nylon 6/CSBR blends. The crystallinity of nylon 6/CSBR blends decreased slightly compared with pure nylon 6, whereas the addition of CSBR powders had little influence on the thermal stability of nylon 6.