This paper designs and synthesizes a series of high-performance waterborne polyurethane (WPU) laminating adhesives using polyester, polyether polyols and isophorone diisocyanate as the main raw materials. It focuses on exploring the effects of polyol types and R value (the ratio of polyol to isocyanate) on the properties of the adhesives, including emulsion viscosity, solid content, water absorption rate of the adhesive film, mechanical properties, and bonding performance on different substrates. The results show that WPU2 with polycarbonate diol (PCDL) as the polyol has the best water resistance and the highest tensile strength; WPU1 with polytetrahydrofuran (PTMG) as the polyol has the optimal elongation at break and exhibits outstanding bonding performance on the polar substrate PET; the regulation of R value can optimize the bonding performance of the adhesive on the non-polar substrate BOPP. This type of WPU laminating adhesive features low VOC emissions, no benzene-based solvents, excellent flexibility, and good resistance to high and low temperatures. It not only meets the environmental protection and safety requirements in packaging fields such as food and medicine, but also shows potential application value in high-end fields like aerospace interior compounding and lightweight transportation structure bonding. Its performance is highly compatible with the strict requirements for materials in the modern aerospace and transportation industries. The adjustable strong adhesiveness, compliance with strict emission standards, and adaptability to various substrates make it an ideal choice for a new generation of composite manufacturing, especially suitable for industrial fields pursuing reliability, sustainability and high performance.