The synthesis of pyrimidine- and pyrazole-based acyclo-C-nucleosides as carbohybrids was optimized and developed. The synthesis of acyclic polyol-fused pyrimidines was achieved in good to excellent yield with high purity by the cyclocondensation of 2-C-formyl glycals and various amidines using K 2 CO 3 as inorganic base in co-solvent system. In comparison, the syntheses of pyrazole-based acyclo-C-nucleosides were accomplished simply by the cyclocondensation of 2-C-formyl glycals with hydrazine hydrate at room temperature and with phenyl hydrazine at refluxing temperature in ethanol.