This　study　highlights　the　innovative　use　of　increased　rare　earth　elements　to　enhance　the　dielectric　properties　of　materials　and　devices.　The　AlOC-129Ln　series,　features　the　highest　number　of　rare　earth　dopants　in　aluminum　oxo　clusters　to　date.　The　trivalent　ions　in　AlOC-129Ln　impart　a　high　dipole　moment,　significantly　elevating　the　dielectric　constant　(k)　of　the　doped　polymer　films.　AlOC-129Ce,　in　particular,　exhibits　the　largest　molecular　size,　which　enhances　interfacial　effects　and　achieves　a　relative　dielectric　constant　four　times　greater　than　that　of　undoped　polymers　and　1.5　times　higher　than　those　with　single　rare　earth　dopants.　The　substantial　molecular　size　(similar　to　2.5　nm)　and　robust　charge　scattering　and　trapping　capabilities　of　AlOC-129Ln　reduce　dielectric　loss　by　up　to　50%　at　high　frequencies.　Additionally,　its　excellent　solution　processability　enhances　breakdown　strength　by　147%,　ensuring　superior　electrical　stability.　This　research　demonstrates　the　versatility　of　the　cluster　doping　strategy　in　effectively　balancing　dielectric　constant　and　loss,　unveiling　the　promising　potential　of　solution-processable　cluster　materials　in　electronic　devices.