To overcome the important challenges of facilitating dehydrogenation in the complex metal hydride, LiBH4, the structural and chemical effects were considered using the strain (-3% - +3%) and five dopants (M = Na, K, Al, F, or Cl). The desorption energies of a hydrogen molecule decreased with increasing tensile strain on the LiBH4(010) surface. The tensile strain was useful for promoting the dehydrogenation process by weakening the B-H interactions. Among the dopants examined, the most favorable dopant to enhance dehydrogenation was Al. The ranking of dopants for hydrogen release was Al > Cl > F > Na > K. Remarkably, codoping of Al and Cl was more effective for hydrogen release than the single doping of Al or Cl with the lowest hydrogen desorption energy. These methods that destabilize metal hydrides are practical for tuning the hydrogen release of LiBH4 hydrides. These studies will provide efficient means for designing excellent hydrides for hydrogen release. (C) 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.