Display omitted Thermosetting urea–formaldehyde (UF) resins as the most common adhesives for wood-based composites emit formaldehyde, which forces producers to lower formaldehyde/urea (F/U) molar ratio for the UF resins synthesis. However, low-molar-ratio (below 1.0) UF resins have low formaldehyde emission at the expense of poor adhesion, which is responsible for the formation of crystalline domains as a result of hydrogen bonds between linear molecules. For the first time, this study reports the conversion of crystalline UF resins to amorphous polymers by blocking the hydrogen bonds, using transition metal ion-modified bentonite (TMI-BNT) nanoclay through in situ intercalation. The modified UF resins with 5% TMI-BNT showed an almost amorphous structure, faster curing and higher cross-linking density compared with those of neat resins, and resulted in 56.4% increase in the adhesion strength and 48.3% reduction in the formaldehyde emission. Thus, blocking hydrogen bonds in low F/U molar ratio UF resins with TMI-BNT converted crystalline UF resins to almost amorphous ones, resulting in a significant improvement in their adhesion with a low crystallinity.