Monocyclic aromatic hydrocarbons (MAHs) are important organic building blocks for the chemical industry, which can be produced by catalytic pyrolysis of biomass. The wide application of bamboo in Chinese industry generates a large amount of bamboo waste which can be utilized as the feedstock to produce MAHs. This study aimed to investigate the effect of bamboo age and bamboo part on the yield of the aromatics by using the Cr and Zn modified HZSM-5 as catalyst. The result showed that the incorporation of metals (Cr and Zn) enhanced the catalytic performance, and the incorporation of Zn was better than Cr. The highest MAHs content (38.67%) and total aromatic content (57.42%) were obtained with the catalyst of 3% Zn/HZSM-5 catalyst at temperature of 400 °C and duration time of 30 min. Younger age (1-year-old bamboo) and the outer skin of bamboo was better for the production of MAHs. This study provided a high value-added application approach for the waste Moso bamboo.