Introduction of high entropy alloys (HEAs) or multi-principal element alloys (MPEAs) in 2004, with their exceptional properties, motivated revisiting conventional alloy design strategies and opened new ways for alloy design and development. Traditionally, HEAs were defined as super-saturated single-phase solid solutions with equal proportions of more than five principal elements. Later, non-equimolar multi-principal compositions also showed great potential, which led to a more relaxed term of MPEA or compositionally complex alloys (CCA), including more multi-phase alloys with “slightly decreased configurational entropy” compared to HEAs. Given the vastness of element/composition combinations, this suggests an astronomical number of alloys waiting to be investigated. Despite significant research efforts since 2004, the potential for new material discoveries using the MPEA concept has hardly been scratched! This offers great potential for new discoveries, but at the same time, it is the biggest obstacle for alloy design since it demands an enormous amount of time and computational capacity. Systematic accelerated metallurgy is an essence to meet the growing demand for developing novel high-performance or multifunctional materials in the industry. This presentation aims to review the challenges, recent progress, and future outlook in accelerated alloy development with a specific focus on high-throughput (HT) screening methods integrated with the Calculation of Phase Diagrams (CALPHAD) technique. A few case studies of alloy development using the HT-CALPHAD will be discussed.