Boron-based materials have been widely studied for hydrogen storage applications. Examples of these compounds are borohydrides and boranes. However, all of these present some disadvantages that have hindered their potential application as hydrogen storage materials in the solid-state. Thus, different strategies have been developed to improve the dehydrogenation properties of these materials. The purpose of this review is to provide an overview of recent advances (for the period 2015–2021) in the destabilization strategies that have been considered for selected boron-based compounds. With this aim, we selected seven of the most investigated boron-based compounds for hydrogen storage applications: lithium borohydride, sodium borohydride, magnesium borohydride, calcium borohydride, ammonia borane, hydrazine borane and hydrazine bisborane. The destabilization strategies include the use of additives, the chemical modification and the nanosizing of these compounds. These approaches were analyzed for each one of the selected boron-based compounds and these are discussed in the present review.