The use of thermal insulation material in building envelopes is closely related to economic benefits, energy-savings, and carbon reduction of buildings. The construction forms of different components in building envelopes have an important influence on the optimization design of thermal insulation in building envelopes. In this study, an integrated optimization approach is proposed to search for the best solution of thermal insulation in external walls and the optimal combination scheme of different construction forms of envelope components in granaries. The integrated optimization approach consists of an orthogonal experimental design (OEDM) method-based determination module of an optimal combination scheme of different construction forms of components, an assessment model-based quantitative analysis module, and an integrated assessment indicator-based selection module of the best solution of external wall insulation. Firstly, the OEDM method is used to determine the optimal combination scheme of different construction forms of the foundation wall of an external wall, thermal insulation material, external window, roof, and floors in buildings. Secondly, integrated economic, energy, and carbon analysis models are developed to analyze comprehensive performance of external wall insulation. Finally, an integrated assessment indicator consisting of an energy balanced index, a carbon balanced index, and weight coefficients is presented to determine the best solution of external wall insulation. The applications of this optimization approach in different ecological grain storage zones in China demonstrated that the outdoor air temperature characteristics could affect the comprehensive performance of external wall insulation in granaries, significantly. The best solution of external wall insulation in granaries in Turpan city, Daqing city, Kaifeng city, Changsha city, Anshun city, and Danzhou city was expanded polystyrene insulation (EPS) with a layer thickness of 0.078 m, 0.048 m, 0.083 m, 0.089 m, 0.062 m, and 0.131 m, respectively. The greatest difference in the lowest entire construction cost and the lowest carbon emission of external wall insulation among different typical climate regions in China was 12.987 USD/m² and 6.3 kgCO2e/m², respectively.