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The absorption peaks observed in the terahertz (THz) region reflect a higher-order structure, crystalline structure, and intermolecular interactions such as hydrogen bonding. Therefore, THz spectroscopy and low frequency Raman spectroscopy are unique techniques for analysing higher-order conformations and intermolecular interactions in semicrystalline polymers. We have investigated changes of the higer-order strucure and hydrogen bondins of several kinds of polymers such as poly(glycolic acid) (PGA), poly-(R)-3-hydroxybutyrate (PHB), polylactic acid (PLA), poly(ε-caprolactone) (PCL), poly (butylene succinate) (PBS), poly (ethylene terephthalate) (PET) and poly (butylene terephthalate) (PBT), and so on by THz spectroscopy and THz Raman spectroscopy with quantum chemical calculations (QCCs).