The combination of alkaline delignification and densification was applied to improve wood mechanical strength. Poplar wood samples were subjected to alkali delignification with varying degrees of lignin and hemicellulose removal followed by hot pressing. Dynamic mechanical performances and dynamic sorption behavior of the untreated and densified wood were then evaluated. Results showed that appropriate removal of lignin can improve the stiffness of densified wood and reduce moisture sorption and the numbers of sorption sites. Fourier transform infrared (FTIR) microscopy along with X-ray diffraction (XRD) were used to explain the viscoelastic and hygroscopicity of delignified and densified wood. Hemicelluloses and lignin were selectively dissolved during alkali treatment. Wood crystallinity was increased after alkali treatment at a moderate concentration of 2%, beneficial to improving the dimensional stability and mechanical performance of delignified and densified wood. The crosslinking of cellulose chains through hydrogen bonding, the decreased content of free hydroxyl groups, and the increased crystallinity in the cell wall contributed to higher storage modulus and lower hydrophilicity. The results support mild delignification and densification as a feasible way towards extending the service life of wood products used as structural materials.