Land resources optimization allocation has great effect on optimizing the industrial structure and distributing the rational productivity. Smart growth is the theory that mainly solves the problem on uneconomical, improvident, inefficient use of land resources in extensive growth and expansion. Thus it can be seen that smart growth can provide a very good guidance to land resources optimization allocation. In view of this, the paper attempted to make a study on land resources optimization allocation based on smart growth in Tongshan, Jiangsu Province. Firstly, on the basis of penetrating analysis of the connotation of the land resources optimization allocation and smart growth, the paper constructed a theoretical framework of land resources optimization allocation based on smart growth. Then, some optioned schemes were obtained by the traditional model of Grey Multi-Goal and Dynamic Programming. Finally, the optimal scheme for land resources optimization allocation based on smart growth was selected by the grey relational analysis method.