This study examines the characteristics of manufactured aggregates by designing an experiment using Mixture Experiments Design of Experiments (ME-DOE) for triaxial whiteware compositions and proposes the optimal mixture for manufacturing artificial lightweight aggregates. The optimal mixture designed using ME-DOE was manufactured in a pilot-scale rotary kiln. The density and water absorption rate of the manufactured aggregates were measured, and the cross-section was observed. Additionally, Mercury Intrusion Porosimetry (MIP) and 3D-CT observation were conducted to observe the pores. The samples designed using the ME-DOE were classified into five types based on the internal microstructure, which had a high correlation with the physical properties of the aggregates. The matrix composition, excluding Fe2O3 and carbon in the area where the black core was created and bloated, was formed in the area of a typical triaxial whiteware mixture. Lightweight aggregates were manufactured at the Pilot Rotary Kiln using a 50:50 mixture of feldspar and ball clay, and the manufactured lightweight aggregates met ASTM C330 standards.