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This paper reports on the development of a tech- nology involving ¹⁰⁰Mo-enriched scintillating bolometers, compatible with the goals of CUPID, a proposed next- generation bolometric experiment to search for neutrinoless double-beta decay. Large mass (∼ 1 kg), high optical quality, radiopure ¹⁰⁰Mo-containing zinc and lithium molybdate crystals have been produced and used to develop high perfor- mance single detector modules based on 0.2–0.4 kg scintil- lating bolometers. In particular, the energy resolution of the lithium molybdate detectors near the Q-value of the double- beta transition of ¹⁰⁰Mo (3034 keV) is 4–6 keV FWHM. The rejection of the α-induced dominant background above 2.6 MeV is better than 8σ . Less than 10 μBq/kg activity of ²³²Th (²²⁸Th) and ²²⁶Ra in the crystals is ensured by boule recrystallization. The potential of ¹⁰⁰Mo-enriched scintillat- ing bolometers to perform high sensitivity double-beta decay searches has been demonstrated with only 10 kg×d exposure: the two neutrino double-beta decay half-life of ¹⁰⁰Mo has been measured with the up-to-date highest accuracy as T_1/2 = [6.90 ± 0.15(stat.) ± 0.37(syst.)] × 10¹⁸ years. Both crystal- lization and detector technologies favor lithium molybdate, which has been selected for the ongoing construction of the CUPID-0/Mo demonstrator, containing several kg of ¹⁰⁰Mo.