Two new compounds, osmjapterpenoid A (1) and osmunjaponin A (2), along with twenty-six known compounds, were isolated from the roots and rhizomes of Osmunda japonica Thunb. The chemical structures of them were elaborated by extensive spectroscopic means, including 1D, 2D-NMR and HR-ESI-MS. Compound 1 is a diterpenoid derived from cembrane with a novel skeleton of 5/13 dicyclic ring system. The possible biogentic pathway of 1 was deduced. Compounds 3 and 26 exhibited moderate inhibition on lipopolysaccharide (LPS)-induced nitric oxide (NO) production in RAW 264.7 macrophages with IC50 value of 32.09 and 19.81 μM, respectively.