Hydrogen bonds are one of the most important directional intermolecular interactions and play key roles in chemical and biochemical systems, but there is still a lack of prediction and understanding of their control. Herein, hydrogen-binding energy (E-HB) acted as a driving force for controllably reconstructing hydrogen bonds with molecular scissors. We related hydrogen-binding energies of the donor-acceptor couple (E-HB,E-2) and the donor itself (E-HB,E-1) and Delta G based on Delta G = a(1)E(HB,1) + a(2)E(HB,2) + a(3). When E-HB,E-1 and E-HB,E-2 satisfy the condition Delta G < 0, the acceptor is predicted as molecular scissors with sufficient reconstruction capacity in breaking the initial hydrogen bonds and forming new ones. Remarkably, we developed an experimental method to determine the E-HB values by a linear equation as a function of chemical shifts (delta) (ln delta + sigma(delta) = -E-HB/RT + A), which is innovational since in the former research E-HB can only be deduced from empirical formulas and DFT calculation. On that basis, the hydrogen bonds of alpha-cellulose were broken and re-formed in molecular scissors-consisting deep eutectic solvents, leading to the white powder transforming into a hydrogel and colorless and transparent thin film materials with distinct crystalline structure, surface flatness, and morphology.