The effects of a three-layer structure and age on the mechanical properties of moso bamboo were investigated. The ages of 1-, 3-, and 5-year-old bamboo were chosen to make test samples, and specimens from each age of moso bamboo were divided into three groups (raw bamboo, bamboo removed from outer layer, and bamboo removed from inner layer) for evaluation of modulus of rupture and parallel-to-grain compressive strength. The regression analysis was completed to evaluate the relationship between mechanical properties and bamboo age. The results showed that the age of moso bamboo was positively correlated with the flexural and parallel-to-grain compressive strengths. The mechanical strength of moso bamboo increased with the increased age of moso bamboo. For the moso bamboo with same age, the flexural and parallel-to-grain compressive strengths decreased for the samples without bamboo outer layer. However, for the samples without bamboo inner layer, the parallel-to-grain compressive strength remained unchanged, but the flexural strength increased. The outer layer of bamboo with high toughness and flexibility played an important role during bending. However, the inner layer of bamboo is relatively brittle, which has negative effects on its flexural strength. These results provide an important basis for the bamboo used in engineering.