Glass spherules have been documented in many geologic deposits and are formed during high-temperature processes that include cloud-to-ground lightning strikes, volcanic eruptions of low-viscosity magmas, and meteorite impacts. This study reviews the known glass spherule–forming processes and proposes, for the first time, a mechanism induced through the heat generated by volcanic lightning in eruptive columns and plumes (laterally spreading clouds) during explosive eruptions. Ash-fall samples were collected from two eruptions where volcanic lightning was extensively documented: the A.D. 2009 eruption of Mount Redoubt, Alaska (USA), and the 2010 eruption of Eyjafjallajökull, Iceland. These samples reveal individual glass spherules ∼50 μm in average diameter that compose <5% of the examined portion of the deposit. Textures include smooth, hollow, or cracked spherules, as well as aggregates, which suggest melting of ash particles as a result of proximity to the electrical discharge channel and subsequent re-solidification of the particles into spherical morphologies. The natural ash-fall samples are compared with pseudo-ash samples collected from high-voltage insulator experiments in order to test our hypothesis that volcanic ash particles can be transformed into glass spherules through the heat generated by electrical discharge. We refer to this new morphological classification of ash grains as lightning-induced volcanic spherules and hypothesize that this texture not only provides direct physical evidence of lightning occurrence during explosive eruptions, but will also increase settling velocities and reduce aggregation of these particles, affecting ash transport dynamics.