The cross-sectional and surface morphologies of highly undercooled bismuth samples are investigated by optical microscopy and scanning electron microscopy. It is found that the grain morphology can be classified into three types. When the undercooling is less than 49 K (49°C), flaky grains with pronounced edges and faces are arranged parallel to each other, showing the feature of lateral growth. When the undercooling is over 95 K (95°C), refined equiaxial grains with several smooth bulges on the surface of each grain are randomly arranged, showing the feature of continuous growth. In the undercooling region from 49 K to 95 K (49°C to 95°C), the features of both lateral and continuous growth are observed. The microstructures within the sample grains obtained at different undercooling regions are dissimilar, but they all show features of anisotropic growth. Based on the critical growth-transition undercoolings, direct expressions that express the relationship between the solid-liquid interface energy and temperature are determined. Homogenous nucleation undercooling is also predicted according to the solid-liquid interface energy obtained from the critical growth-transition undercooling. The predicted results of homogenous nucleation undercooling for bismuth are in good agreement with the experimental results.