Wood is a viable alternative to traditional steel, cement, and concrete as a structural material for building applications, utilizing renewable resources and addressing the challenges of high energy consumption and environmental pollution in the construction industry. However, the vast supply of fast-growing poplar wood has bottlenecks in terms of low strength and dimensional stability, making it difficult to use as a structural material. An environmentally friendly acrylic resin system was designed and cured in this study to fill the poplar cell cavities, resulting in a new type of poplar laminated veneer lumber with improved mechanical strength and dimensional stability. The optimized acrylic resin system had a solid content of 25% and a curing agent content of 10% of the resin solid content. The cured filled poplar veneer gained 81.36% of its weight and had a density of 0.69 g/cm3. The static flexural strength and modulus of elasticity of the further prepared laminated veneer lumber were 123.12 MPa and 12,944.76 MPa, respectively, exceeding the highest flexural strength required for wood structural timber for construction (modulus of elasticity 12,500 MPa and static flexural strength 35 MPa). Its tensile strength, impact toughness, hardness, attrition value, water absorption, water absorption thickness expansion, and water absorption width expansion were 58.81%, 19.50%, 419.18%, 76.83%, 44.38%, 13.90%, and 37.60% higher than untreated laminated veneer lumber, demonstrating improved mechanical strength and dimensional stability, significantly. This method provides a novel approach to encouraging the use of low-value-added poplar wood in high-value-added structural building material applications.