Natural bamboo fibers have attracted growing demands in textile industry due to benefit from their excellent properties and renewable and abundant resource; however, there are still limitations for their application in textile industry because of their poor quality. For this reason, enzymes treatments on mechanochemically modified natural bamboo fibers were conducted to extract noncellulosic matters from finer natural bamboo fibers in this paper. Four enzymes, pectin lyase, xylanase, laccase, and cellulase, were used to remove pectin, hemicellulose, lignin and to loosen the compact structure of fibers, respectively. Furthermore, the concentrations of four enzymes were optimized in terms of fiber chemical composition, weight loss, fineness, and tenacity to obtain high quality fibers. An obvious reduction in amount of noncellulosic substances and also a remarkable improvement in fineness in the modified fibers can be found from the experimental results. The optimum parameters are determined as: 0.6 % pectin lyase, 1.2 % cellulase, 0.3 % xylanase, and 1.2 % laccase; and the natural bamboo fiber thus obtained is 77.51 % in cellulose content, 2.81 tex in fineness, and 2.62 cN/dtex in tenacity.