This paper describes the research on the materials and design methods for advanced smart radiator devices (SRDs) on large-area flexible substrates utilized on spacecraft. The functional material is thermochromic vanadium dioxide. The coating design of 3RD is similar to the design of broadband filter coatings in a mid-infrared region. The multilayer coatings have complex structures. Coating materials must be highly transparent in a required spectrum region and also mechanically robust enough to endure the influence from the rigorous environments of outer space. The number of layers must be very small, suitable for the deposition on large-area flexible substrates. All the coatings are designed initially based on optical calculation and practical experience, and then optimized by the TFCALC software. Several designs are described and compared with each other. The results show that the emittance variability of the designed SRDs is great than 400%, more advanced than the reported ones.