ABSTRACT Bamboo exhibits remarkable flexibility and bent shape stability in thermal-bending. To explore how bamboo responds to bending, this study investigated the chemical properties on the concave, middle and convex walls (marked as CW, MW, VW respectively) of bent bamboo Phyllostachys iridescens though XRD, XPS, and FTIR analyses. Results indicate a reduction in crystallinity from 42% of MW to 39% of CW and 40% of VW. Notably, the peak shifts of CW and VW indicates the neutral layer on CW and VW experience an offset toward the convex surface. Chemical degradation varies on the thermal bent bamboo sections, the O/C ratio increases from 0.26 of MW to 0.36 of CW, accompanied a decrease in the Cox/unox ratio from 0.93 of MW to 0.81 of VW. This indicates that VW undergoes more significant degradation of cellulose and hemicelluloses, while CW experiences a greater loss of extracts. Additionally, FTIR analysis indicates that the ester bond peak at 1731 cm−1 flattens on CW, while it splits into two peaks on VW, with one of the peaks shifting to a higher wavenumber of 1735 cm−1. This suggests a reduction in the intermolecular distance between lignin and hemicelluloses on CW, whereas a higher lignin content and compression stress on VW.