Aerogels have garnered extensive attention as crucial materials in the field of engineering. In this study, 2,2,6,6-tetramethylpiperidinyl-1-oxid (TEMPO)-oxidized bamboo cellulose nanofibril (TOCNF) was introduced as a critical component into the crosslinking network of polyvinyl alcohol (PVA) using glutaraldehyde (GA) as a bridge to obtain aerogel with enhanced pore structures and mechanical properties. The properties of composite aerogels with different TOCNF additions were investigated. The results showed that the aerogels exhibit low density, excellent pore structure, outstanding thermal stability and mechanical properties. The compressive strength and modulus of elasticity of the aerogel with 1.5% TOCNF had significantly increased by 260% and 150%, respectively, compared with blank sample. Furthermore, the aerogel displayed robust stability in liquids due to the interaction between TOCNF and PVA forming a crosslinked network structure. This work demonstrates a bamboo cellulose nanofibril enhanced aerogel that can be widely applied in the fields of energy, adsorption, construction, thermal insulation, and so on.