To　achieve　high　concentration　of　Ce3+　ions　in　Gd3Fe5O12　(GIG)　crystal,　the　structure　of　codoped　Sc3+　and　Ce3+　ions　was　designed　and　the　doping　energy　was　evaluated　by　the　firstprinciples　density　functional　theory.　Based　on　this,　Ce,Sc,Ca:GIG　crystals　with　centimeter　size　and　good　quality　were　successfully　grown　by　an　improved　edge-defined　film-fed　growth　method.　The　transmission,　magnetism,　and　magneto-optical　effects　were　investigated　in　detailed.　The　Ce-doped　concentration　as　high　as　18　at%　results　in　the　(Ce0.54Gd2.41Ca0.05)　(Sc0.45Fe4.55)O12　crystal　having　excellent　magneto-optical　properties.　Its　Faraday　rotation　angle　increased　to　about　-1534　deg.　cm-1　at　l　=　1550　nm.　Therefore,　the　excellent　magneto-optical　performances　reveal　that　Ce,Sc,Ca:Gd3Fe5O12　crystal　has　great　potential　to　be　utilized　for　miniaturized　and　high　performance　optical　isolators　in　1550　nm.(c)　2022　The　Author(s).　Published　by　Elsevier　B.V.　This　is　an　open　access　article　under　the　CC　BY-NC-ND　license　(http://creativecommons.org/licenses/by-nc-nd/4.0/).