This paper reports on the development of a technology 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 ( ∼1kg ), high optical quality, radiopure 100Mo -containing zinc and lithium molybdate crystals have been produced and used to develop high performance single detector modules based on 0.2-0.4 kg scintillating 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 10μBq/kg activity of 232Th(228Th) and 226Ra in the crystals is ensured by boule recrystallization. The potential of 100Mo -enriched scintillating bolometers to perform high sensitivity double-beta decay searches has been demonstrated with only 10kg×d exposure: the two neutrino double-beta decay half-life of 100Mo has been measured with the up-to-date highest accuracy as T1/2 = [6.90 ± 0.15(stat.) ± 0.37(syst.)] ×1018years . Both crystallization 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 .