We report on the development of scintillating bolometers based on lithium molybdate crystals that contain molybdenum that has depleted into the double-βactive isotope100Mo (Li2100deplMoO4). We used two Li2100deplMoO4cubic samples, each of which consisted of 45-millimeter sides and had a mass of 0.28 kg; these samples were produced following the purification and crystallization protocols developed for double-βsearch experiments with100Mo-enriched Li2MoO4crystals. Bolometric Ge detectors were utilized to register the scintillation photons that were emitted by the Li2100deplMoO4crystal scintillators. The measurements were performed in the CROSS cryogenic set-up at the Canfranc Underground Laboratory (Spain). We observed that the Li2100deplMoO4scintillating bolometers were characterized by an excellent spectrometric performance (∼3–6 keV of FWHM at 0.24–2.6 MeVγs), moderate scintillation signal (∼0.3–0.6 keV/MeV scintillation-to-heat energy ratio, depending on the light collection conditions), and high radiopurity (228Th and226Ra activities are below a few µBq/kg), which is comparable with the best reported results of low-temperature detectors that are based on Li2MoO4using natural or100Mo-enriched molybdenum content. The prospects of Li2100deplMoO4bolometers for use in rare-event search experiments are briefly discussed.