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In the crystal research the areas between different grains have great effect on the mechanic, metallurgy, corrosion properties to the material. We call these areas grain boundary. People put great emphasis on them and have tried many methods to research them. The grain boundary has high energy and the energy value is changed with the orientation. Finding the law between them can deepen the material research. The universal grey set is a set of universal uncertain information which includes all uncertain information (random, fuzzy, uncertain and grey etc). Now many scholars have put it into different fields. In the paper the authors firstly put the universal grey uncertain systems into the grain boundary and establish the relationship of energy and orientation. The fitting data and predictive data are good. The model is fit for equal and unequal interval and is deserved to be used into other engineering problem.