Five-fold symmetric diamond crystals（FSDCs） were synthesized by hot filament chemical vapour deposition（HFCVD） methods. Their surface morphologies and defects were characterised by scanning electron microscopy（SEM）. From the perspective of nucleation-growth, a growth mechanism for icosahedral and other five-fold symmetric diamond crystals was discussed. Computer modelling was also carried out. The results show that the dodecahedrane（C20H20） molecule is proposed as a nucleus for the growth of icosahedral diamond crystals（IDCs）, wherein the 20 {111} surface planes develop orthogonal to the direction of the original 20 C—H bonds by sequential H abstraction and CH3 addition reactions. IDC can be pictured as an assembly of isosceles tetrahedra, with each tetrahedron contributing a {111} plane to the surface of the IDC and the remainder of the tetrahedral surfaces forming twin planes with neighbouring tetrahedra. The small mismatch（1.44°） between the {111} surface dihedral angle of a perfect icosahedron and that of a twinned icosahedron reveals itself via twin planes in the IDC grain. The modelling suggests how the relief of strain induced by this distortion could lead to the formation of defects such as concave pentagonal cavities at vertices and grooves along the grain edges that accord well with those observed experimentally. Similar arguments based on growth from the hexacyclo pentadecane（C15H20） nucleus can also account for the observed formation of star and rod shaped FSDCs, and some of their more obvious morphological defects.
