In summary, we combined simulations, data mining, and design principles to propose bi-selective OSDAs for intergrowth zeolites. By visualizing the OSDAs according to their phase competition and shape matching metrics, we designed promising bi-selective candidates for cost-efficient synthesis of intergrowth zeolites. The method was demonstrated for small-, medium-, and large-pore zeolites, and extended towards several known intergrowths. Furthermore, we proposed OSDAs that could realize a hypothetical intergrowth. This work is expected to accelerate discovery of intergrown zeolites using computation. of organic structure-directing agents for zeolites using nature-inspired ant colony optimization. Chemical Science 2020, 11, 8214-8223.