Thermoelectric　materials　hold　great　potential　for　direct　conversion　of　ubiquitous　waste　heat　into　electricity.　However,　their　commercialization　is　hindered　by　low　efficiency,　reliance　on　rare　and　expensive　Te,　and　limited　stability　under　operating　conditions.　This　review　explores　recent　advances　in　novel　strategies　for　achieving　high　thermoelectric　performance　and　stability　in　Te-free　inorganic　bulk　materials.　First,　we　discuss　diverse　innovative　techniques　aimed　at　substantially　enhancing　electrical　transport　properties.　These　methods　encompass　strategies　such　as　charge　carrier　engineering,　band　convergence,　band　inversion,　valley　anisotropy,　multiband　synglisis,　and　the　incorporation　of　resonant　levels　or　midgap　states.　Then　we　focus　on　strategies　to　reduce　lattice　thermal　conductivity,　including　phonon　scattering　induced　by　multidimensional　defects,　off-center　doping,　resonance　scattering,　and　lattice　softening.　Additionally,　this　review　presents　strategies　for　decoupling　electron　and　phonon　transport　to　enhance　the　thermoelectric　performance　of　materials　further.　The　strategies　include　interface　engineering,　crystal　symmetry　manipulation,　high-entropy　engineering　and　nanostructuring,　high-pressure　technology,　and　magnetically　enhanced　thermoelectrics.　Moreover,　we　highlight　novel　strategies　for　improving　the　chemical　and　thermal　stability　of　materials　under　operating　conditions.　Last,　we　discuss　current　controversies　and　challenges　and　suggest　future　directions　for　further　research　to　improve　the　thermoelectric　performance　of　Te-free　bulk　materials.　©　2025　American　Chemical　Society.