Paper grade bamboo pulp with high molecular weight was irradiated in air by 60Co γ-ray to improve its dissolving property in N-methylmorpholine-N-oxide monohydrate (NMMO·H2O). The effects of γ-ray radiation on the structure and properties of the bamboo cellulose were investigated. The results showed that the bamboo cellulose with a G(s) value of 0.94 μmol J−1 was easily degraded by the 60Co γ-ray radiation. When the radiation dose increased, the average degree of polymerization () of bamboo cellulose was decreased and its molecular weight distribution (MWD) became narrow, while its crystalline structure did not change obviously. Consequently, a spinning dope with high cellulose concentration and good spinnability was obtained in the range of absorbed dose from 5 to 10 kGy. This work presented an economic method to prepare regenerated bamboo cellulose fiber from paper grade bamboo pulp.