In summary, we have developed a computational framework for systematic optimization of the transport properties and dopability of thermoelectric alloys. We simultaneously consider the effects of alloying on electronic and thermal transport, and dopability, which makes this computational framework unique compared to other computational studies of thermoelectric alloys. We apply this framework to identify the optimal compositions of n-type Ba 2(1 x) Sr 2x CdP 2 Zintl thermoelectric alloys by achieving conduction band convergence, minimization of alloy scattering of electrons, lowering of k L , and ensuring n-type dopability. Our computational framework can be used to accelerate the design of thermoelectric alloys with desired transport and doping properties. Such a framework can be used to design alloys for other functional applications beyond thermoelectrics.