The dramatically increasing computing capability of modem supercomputers allows people to explore the properties of thousands of potentially useful materials in a fraction of time that the real experiments might take.This makes rational design of the functional materials with desired properties in computers come true.In this paper, if time allowed we would present four aspects of results on computational design of optoelectronic materials by using either the intelligence-based structure searches or the high-throughput calculations: (i) Optimizing Si quantum well systems to achieve the large enough valley splitting for reliable Si-based quantum computing[1];(ii) Designing the direct band-gap materials based on the heterostructures built from the layered group-VIB transition metal dichalcogenides[2,3];(iii) Exploring the possibility of the ternary oxide materials containing Sn2+ being p-type transparent conductors;(iv) Seeking for new-type organic-inorganic hybrid perovskite materials for solar cell applications.