Driven　by　materials　science　development,　the　thermoelectric　performance　has　been　enhanced.　However,　only　increasing　the　figure　of　merit　to　enhance　the　thermoelectric　efficiency　becomes　more　challenging.　Here,　we　combine　an　enhanced　figure　of　merit　and　geometry　optimization　of　a　device　by　computer-aided　design　to　achieve　a　record-high　thermoelectric　efficiency　of　16%.　A　figure　of　merit　over　2.2　in　p-type　Ge1-x-yCrxSbyTe　alloys　is　achieved　resulting　from　the　convergence　of　three　valence　edges　induced　by　Cr　doping　to　enhance　the　power　factor　and　superlattice　precipitates　to　lower　the　thermal　conductivity.　Using　finite　element　analysis　simulations,　we　optimize　the　geometry　of　a　segmented　thermoelectric　device　made　of　the　as-developed　Ge1-x-yCrxSbyTe　and　other　reported　materials,　leading　to　a　record　high　efficiency.　Furthermore,　our　simulations　on　over　70　existing　n-type　thermoelectric　materials　can　serve　as　a　library　to　bridge　the　gap　between　materials　science　and　device　engineering　to　achieve　high-efficiency　thermoelectric　devices.