Taking the urban districts of Hohhot as the study area, using the classification data of land use change and relevant socio-economic statistical yearbook data in 2001-2016, taking the dual targets of economic-ecological and related constraint factors as the optimal decision of optimization of land use structure, using the Grey Multi-objective Programming (GMOP) and Genetic Algorithm (GA) to estimate the intervals of predictive threshold value of the factors and inequality constraint equations, and on the basis of it to designed two schemes for optimization of land use structure for the study area in 2030 and made them in comparison and optimization. The results show that in contrast to the primitive land use structure, the optimized scheme based on the economic-ecological comprehensive benefit is better than the current land use structure as the two aspects of the overall land output benefit and the scale combination of single type land use and the current land use structure.