Geopolymer　cold-bonded　aggregate　(GCBA)　is　a　new　artificial　aggregate　manufactured　by　agglomeration　of　aluminosilicate　precursor　powder　hardened　by　alkali　activation.　This　paper　presents　a　multi-objective　material　design　procedure　for　GCBA　based　on　the　simplex　centroid　design　method,　using　metakaolin　(MK),　fly　ash　(FA),　and　silica　fume　(SF)　as　the　ternary　precursor　materials.　Based　on　the　test　data　from　10　groups　of　GCBAs　with　designed　compositions　and　response　surface　models　established　thereby,　the　optimal　composition　domain　of　the　precursors　was　determined　and　experimentally　validated.　The　effect　of　the　precursor　composition,　especially　the　content　of　SF,　on　the　performance　of　GCBA　was　evaluated.　Results　showed　that　in　the　optimal　composition　domain　of　the　precursor　(36–48　wt%　of　MK,　33–46　wt%　of　FA,　and　15–24　wt%　of　SF),　the　developed　GCBA　achieved　the　given　high-performance　targets　of　bulk　crushing　strength　higher　than　21.0　MPa,　the　loose　bulk　density　less　than　1200　kg/m3,　and　water　absorption　less　than　10%.　SF　content　(Si/Al　ratio)　has　a　great　influence　on　the　performance　of　GCBA:　a　suitable　amount　of　the　incorporated　SF　(Si/Al＜1.7)　promoted　the　formation　of　K-A-S-H　gels　in　GCBA,　leading　to　an　increase　in　strength　and　density,　and　a　decrease　in　water　absorption;　while　excessive　SF　(Si/Al＞1.7)　induced　a　self-foaming　reaction,　resulting　in　a　porous　microstructure　and　reduced　strength　and　density.　©　2023　The　Authors